think I can contribute a lot here.
Divergence Eve: I actually find this anime to be really good and have large boobs. It is basically a fairly realistic Sci-fi about a team of female pilots trying to safe guard a space station. The science and lore is fairly in depth. Even though it has a sizable helping of fan service and some light hearted scenes, this is actually a rather dark and moving anime. I found myself caring a lot for the characters and felt the emotions when characters died. Over all its a intense anime that doesn't bank on its fan service. My two complaints for it is the CG could be much better, and a majority of intro/endings really are not appropriate for the series. The first half of the series intro is great and sets the mood well. The ending credits and the intro are way to j-pop goofy for whats going on. There be times when a episode would end with someone die or things looking grim, just to be slammed with a upbeat fanservice fest. Its emotional drops the clutch to change gears. If you like intense Sci-fi with boobage sprinkled in for added flavor, definitely check it out.
Grenadier: This series is a lot of fun with some thoughtfulness in it. This anime is about a Gunslinger woman (who is well endowed) going around doing what gunslingers do best. The main character somewhat comes off as a female Vash the Stampede. Very goofy, innocent, attempts to promote peace, and all round bad ass. She also has this neat trick were she store her extra ammo in her cleavage, and when in need to reload her gun, gives them a good bounce, twirls, and catches the round in her revolver. Nice! Over all, this anime is alright. I think it tires a tad to hard to put the fan service in the anime, but strangely, it ties in rather well to the theme and message the anime tries to convey. Over all, I really enjoy this anime and is well worth checking out.
Desert Punk: If you want to expand your boob vocabulary and do so while watching a good anime, this is the anime for you. This is anime is set in a post-apoc world that is focused on a main character that very well defines the true neutral alinement. This small guy uses trickery, wit, and intelligence to defeat his foes. Unlike like other heros thou, this one is very much a anti-hero. He is fairly vulgar, self interested person, who possess a very questionable morality. Oh and he loves breasts, enough maybe to even rival this forum. This results in a lot of his comic foil. There is also a female character who has a really big and nice pair, which she knowingly utilizes to manipulate men and the main character. Over all this is actually a really good anime. I would recommend the dubbed version because it is well executed and the banter is very enjoyable.
Witchblade: This is a anime about a single mother trying to care for her **09** while fending off supernatural assassins. This is set in a modern world where certian women are in possession of a weapon called a witchblade, which turns them in to killing machines. A good deal of the women, including the main character, are large breasted, and when in witchblade mode, ramp up the sexy. Over all, i think this is a fairly decent anime. Aside the fan service, this anime does a good job making very likeable and fairly realistic characters. You can really feel the affection that is between the main character and her daughter, despite her short comings. I say this anime is well worth the watch. Its a fun, fairly deep anime, that doesn't over due its fan service.
Well there are some animes that I can think of for right now. There area ton of animes with huge boobs, but unfortunately are fairly crappy. I like fan service as much as the next guy, but when its all a anime focuses on, then it becomes a annoying waste of time. If i come across other "good" animes with large breasts, I'll do my best to share them with you folks. I hope folks enjoys these shows as much as I have.