I think Zetsubou Sensei was their first big hit. There's a reason they got 2 sequeals and several OVAs out of it. Kodi Kumeta's acidic humour and simple art style and Shafts humourous insertions and propensity for visual weirdness went together hand in glove.
How well Shaft does related entirely to how well the source material relates their style (as Child of Sierra said). Bakemonogatari and SZS are good examples of this.
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