The first thing I looked at was the gender breakdown on these sites. I got all of the information being presented not from browsing the sites themselves, but rather by using Google's AdPlanner feature and recording the traffic statistics they supply. The gender breakdown is probably most important to people seeking a partner of the opposite sex as it plays a big role in how much you will stand out amongst the other people a potential partner may be searching on these websites. Here were my results (Click to see full size):

Ignoring the male specific website GayRomeo.com for the moment, the free online dating service OKCupid.com had the largest proportion of males to females with 64% of visitors to their website being recorded as male. On the flip side, the website Zoosk.com had the largest female to male ratio with 59% of visitors being recorded as female.
More shocking than the gender split between the websites was the diversity in educational level of visitors to the sites. I recorded the percentage of users who had received a bachelor's degree or above as a good measure of educational level, and surprisingly the results varied by as much as a factor of 5.

The two best educated dating sites also happened to be the male-heavy ones with OKCupid.com coming in at 37% of visitors having a bachelor's degree or above and GayRomeo.com coming in with 34%. On the flip side, there were quite a few services with absolutely abysmal education numbers. Mate1.com had only 9% of its visitors recorded as having a bachelor's degree or above, while True.com was recorded with a mere 7%.
The final piece of information I gathered was the sheer number of unique visitors coming to each website every day. If you are looking for a very specific sort of someone, then your chances of being able to find that sort of person are much better if you have a lot more people to choose out of.

Match.com seems to be far and away the most used online dating service with PlentyOfFish.com still living up to its name.
Taking all of these factors into account I'd recommend OKCupid.com as the best option for adrophiliac (meaning attracted to adult men) users with GayRomeo.com being a close second for male androphiliacs. For gynephiliacs (meaning persons attracted to adult females) I would suggest Match.com as the best option if you are willing to pay for a dating service, and PlentyOfFish.com as the best option for a free dating service. For female gynephiliacs looking for a well-educated crowd, OKCupid.com would also make an excellent option despite the somewhat smaller population.