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A growing interest in the development of thick functional structures with high aspect ratio for microelectromechanical system (MEMS) applications has triggered the investigation of several polymer materials. This paper presents LF55GN flexopolymer material as a new negative-tone photoresist to fabricate ultrathick MEMS microstructures. Up to 4-mm-thick layers are obtained using a casting method in a single photolithography step. Standard UV illumination is used to polymerize such thick microstructures in less than 1 min and with an aspect ratio up to 27. We have fabricated microstructures on rigid, flexible, and stepped substrates. Using oblique UV exposure, tilted pillars are achieved with an angle of 25deg to the substrate normal. Due to the elastomeric nature of the LF55GN flexopolymer, the microstructures can be easily deformed without causing any stress-related problems.