LiIon batteries can be safely (enough) charged at the rate advised by their manufacturers. Faster may be possible and may be "safe" but all guarantees are off and shorter life or instantaneously very short life are definite options.
Added last. This table from the battery university reference below provides excellent comment on LiIon charging times.

The manufacturer specified maximum charge current is C/1 (= 1A per Ah of capacity) but some specify C/2, a few 2C, and some specialist cells may allow much higher charge rates.
This current is applied until Vmax is reached - typically 4.1 or 4.2 V.
This voltage is maintained and the battery draws decreasing current under its own "control" until a charge termination decision is made.
Under constant current ramp up Vmax is reached at about 66% to 85% of full capacity - probably typically around 80%? At 1C 80% of capacity is reached in 80% of 1 hour = 48 minutes. SOME fast chargers declare charging complete here- so some may seem very fast without doing anything clever except stopping early.
This is the optimum storage point for long life.
Current will now ramp down towards zero in a non linear fashion under battery chemistry control. The lower it gets the slower it goes. Some chargers will terminate charging at say 33% of full current, or 25% or 20% or 10%. To get maximum possible capacity the current must be allowed to fall to a low % of max so can take much longer than the time taken to put in the first 80% or so. So some chargers may stop at say I=33% of max and take 2 hours all up, and others may stop at 10% of Imax and take 4 hours - and all may be close to identical in general principles.
Due to the slow decreasing-current tail being an essential part of a truly full charge, doubling the Imax to say 2C will only make charging somewhat faster due to long decreasing-current tail.
Here's a better than usual comment on LiIon charging.
Battery University - Charging Lithium Ion Batteries
Text from there - note comments on "miracle chargers".
The Li‑ion charger is a voltage-limiting device that is similar to the lead acid system. The difference lies in a higher voltage per cell, tighter voltage tolerance and the absence of trickle or float charge at full charge. While lead acid offers some flexibility in terms of voltage cut‑off, manufacturers of Li‑ion cells are very strict on the correct setting because Li-ion cannot accept overcharge.
The so-called miracle charger that promises to prolong battery life and methods that pump extra capacity into the cell do not exist here. Li-ion is a “clean” system and only takes what it can absorb. Anything extra causes stress.
Most cells charge to 4.20V/cell with a tolerance of +/–50mV/cell. Higher voltages could increase the capacity, but the resulting cell oxidation would reduce service life. More important is the safety concern if charging beyond 4.20V/cell. Figure 1 shows the voltage and current signature as lithium-ion passes through the stages for constant current and topping charge
http://batteryuniversity.com/learn/article/charging_lithium_ion_batteries

There are new lithium based chemistries and new mechanical arrangements which allow lithium based cells to be charged at faster rates. If the manufacturer says it is so it indeed may be. I've seen apparently standard LiIon cells with 2C charge ratings but the norm is 1C max. (see above)
A major factor in lithium Ion lifetime and rate problems is the significant change in mechanical volume as Lithium metal gets added to or taken away from portions of the cell. Such issues are a significant factor in establishing LiIon cycle lifetimes. One attempt to improve this involved making a structure which remained in place when the lithium plated in and out giving mechanical stability. This lead to a reduction in available capacity die to soace being taken by the structure, and other effects lead to a reduction in maximum terminal voltage BUT gave us the Goodenough (great name) battery aka liFePo4 with about 60%+ the capacity and 15% less terminal voltage and vastly more longevity and more robust electrical characteristics. [Goodenough is easier to remember than the actual inventor Akshaya Padhi - a membr of Goodenough's research team).
Goodenough interview 2001 !!! Wow !!!
Don't even think about creating the setup you just described. It is bloody dangerous.
If you wire the "solar cell pack" and the two battery packs in parallel without connecting the Raspberry Pi, you'll get a loop. Kirchhoff's second law explains that the sum of voltages around a loop must be zero. In this case, if you start going around the loop in one direction, you'll encounter the two power sources with opposite directions, so now their difference must be zero - so they must be at an equal voltage. Will this be 6V (dictated by the solar panels) or 3.7V (dictated by the battery packs)? The following will happen:
- Initially, without sunlight, the common voltage will be 3.7V. No current flows, since the solar panel does not let current flow backwards (its resistance goes near infinity). All is well for now.
- Then you apply sunlight. The solar panels try to increase the voltage to 6V, but at this voltage the batteries would allow through much more current than they can supply. So the panels drop their voltage to 3.7V, but still begin to charge the batteries with the couple hundred milliamps they can supply, until the voltage in the battery packs reaches 6V. And there's a pretty good reason the batteries are rated at 3.7V.
- If I learned anything about Li-ion and Li-polymer batteries is that they are very easy to upset. And they especially don't like being overcharged. If they are indoors, they will blow up your desk and burn your house down. If they are oudoors, they'll happily ignite the grass around them. Then burn your house down. Li-ion and Li-polymer batteries are not toys. Don't even think about putting them in a circuit where there's even a slight chance they'll get overcharged.
Connecting the Raspberry Pi before the detonation wouldn't work out well either. The 3.7V combined power supply is not enough for the Pi, which will then do one of the following (I'm not familiar with the Pi's power supply circuit):
- Pull a lot of current overheating the battery, the solar panel and maybe even its own on-board voltage regulator. It will not boot, or even if it does, it will frequently crash and reboot because of the inadequate voltage. This goes on until one of the components fail: if it's the solar panel, you're safe. If it's the Pi, it's the time bomb scenario all over again. The battery packs also don't like being over-discharged, but as far as I know, they don't burst out in flames then. They just don't work anymore.
- Don't pull any current at all. Then it's like you didn't connect it at all. Time bomb again.
Creating a circuit which safely combines solar and battery power requires advanced electronics skills and dedicated circuitry. In your case, I would follow S.J. Becker's advice (+1) and buy a (solar powered) power bank from eBay. The circuitry is there, pre-made for you and it can power your Raspberry Pi longer than your setup would have even if it worked. I know they are not as cheap as using things from your parts bin, but they are definitely cheaper than replacing your burnt furniture.
Additionally, does the thing have to be solar powered?
Edit: Some battery packs have built-in protection circuitry that shuts the power off if the battery is overcharged, so there's a chance your setup won't actually ignite but just not work at all.
Best Answer
Batteries made by Yardley Lithion
Well discussed here:
Life verification of large capacity Yardney Li-Ion cells and batteries in support of NASA missions
One version 60% capacity after 3000 cycles deep discharge
Another - 25,000 cycles, 40% depth of discharge 35 min charge/discharge periods (LEO satellite simulation). Max Voltage = 3.8V/cell!
Next Generation and Domestically Produced Active Materials for Lithium-Ion Cells for Military and Aerospace Applications
Adding material from comments that increases usefulness of answer
PJC in Jan 2013 noted that majopr points from the paper cited above included
and
" ... also to keep the rate and depth of discharge low ("battery could not support rate of discharge >C/2 at -20C when <75% charged after 1010 sols of operation"), and for long term storage to keep the batteries at 50-70% charge, not fully charged."
He also noted - The anode composition and surface coating may also be different from consumer batteries.