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Eve no Jikan is the it. Nothing comes close to the quality of storytelling from every aspect of what makes an anime, anime. That said, Negima OVA didn't receive much attention despite some really good animation works along with some semblance of stories put together. The story is still scatter-brain effort, but it still plays better compared to the TV series. Hellsing has also released OVA series though it's not as hush-hush as Negima. Difference from the TV series is that the OVA is truthful to the manga counterpart. Hellsing OVA is still ongoing. There is another one that came out recently which is called Koi Sento by Sunrise. It's not bad. Sunrise tries their hand out on the effervescent 3D technology that is more prevalent these days. Freedom OVA is another one that also employs the 3D technology. The story is actually one of my favorite and I feel the show didn't get as much attention as it should have. Isekai no Sekishi Monogatari is a 13 episode OVA series which follows the classic Tenchi style of storytelling. Black Lagoon has also an ongoing OVA series at the moment where it focuses on the awesome Roberta who doesn't think twice about blowing someone's head off. She is on drugs too! Denpa Teki Kanojo is another two episode OVA. It incorporates murder mysteries with High-School setting. I don't have much of an opinion on it. Bungaku Shoujo is another OVA that I've enjoyed a lot, mostly for the plot. The animation is average, but the plot itself is more than enough to capture potential audience. Kowarekake no Orgel is a one episode OVA with a pretty good story. The story is... well... I don't want to give it way. Kyou No Go Ni was another OVA based on elementary/middle school setting. The show is comedy with come-of-age in mind. The subsequent TV series pales in comparison to the OVA.
I'm sure there are many other ones that I'm missing. Like there is one OVA that is on the tip of my tongue that I can't think of the name of at the moment. I'll add it if it comes back to me.
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