This is a tough one. I think I will have to re-watch 3.0+1.0 a few more times, and possibly marathon all 4 movies in 1 session to REALLY nail it down.
Currently I think I have to go with:
#1 1.11 It didn't break any new ground, but it was a lovingly and perfectly executed re-build (as the title says!) of the first third of NGE, with the same story (with a few cryptic hints tossed in) laid overtop a MASSIVE re-making of the animation quality of those episodes of NGE that it covered. All the little details were lovingly and carefully re-done and expanded upon, and included some wonderful CGI work compared to later movies. (Ugh that Rei head in 3.0+1.0)
#2 3.0+1.0 While it wasn't completely what I was hoping for, it concluded the series in a far more satisfying manner then Eps 25+26 of NGE or EoE ever did. Much was explained although too much was still untouched upon, but this leaves room for a possible 2.5 sometime in the future to cover the time-skip. It also fairly conclusively lays down the fact that Rebuild was not so much a remake or sequel to NGE+EoE, but a continuation and looping story that involved constant failures to 'get it right' as we witnessed in EoE, but this time they got it right by humanizing Shinji before throwing the final choice at at him, and he makes the right decisions to conclude the cycle in triumph.
This movie might become #1 in time, but there were enough complete howlers (Friggin 20 year old Final Fantasy Spirits within had better facial texturing and animation then the goddamn giant Rei head in this movie, not to mention the immersion-breakingly stupid looking skull-head Eva Infinities) and confusing segments to push it down to #2 for now.
#3 2.22 While high quality overall, there were a few very bad animation choices. Especially in the climactic battle with Zeruel where he not only sent out jaws and presumably an everted stomach about 3 football fields long to crunch down on Rei's Eva, the volume of high-pressure LCL that shot out of the remaining boots would have embarassed Yoshihiro Mishimura. (Tokyo Gore Police) Also with the exception of Mari and the Tagbtha Base segment, it also didn't break much new ground until the end when everything completely went off the rails, setting up the clusterfuck that is:
#4 3.33 The timeskip threw out damn near everything we expected (which was the point) and subverted expectations so hard with introducing a 14-year timeskip, new characters, a new mega-powerful flying Battleship and complete and utter confusion about just what the hell went on after Unit 1 was stopped by a spear thrown by a man from the moon. It was also extremely mean-spirited in almost every way with everyone treating Shinji like a leper who was rolled into a den of skunks and not telling him a damn thing, when almost everything that happened in the rest of the movie would not have happened if Misato and the rest of the Wunder crew acted like human beings and filled him in on his obvious confusion. Either way, it was an awful way to handle the timeskip and while suitably apocalyptic at the end, was still unsatisfying overall.
Okay, that's enough typing. time for Sunday breckie!
"Yes ladies and gentlemen, in France Asuka swears like a sailor and confirms that she's the butch of her apparent lesbian relationship with Mari, Mari insults people that ignore her, and Shinji Ikari tells to Sakura Suzuhara and Misato Katsuragi to go fuck themselves!" -ElMariachi