Core–shell PMMA–Au nanocube structures made by a combination of nanoimprint lithography and sidewall deposition were used as template for electrodeposition of MoS2, Ni, and Pt. Linear sweep voltammetry experiments obtained in an aqueous solution containing 0.29 M H2SO4 (pH 0.24) showed that the onset potential of the core–shell–shell PMMA–Au–MoS2 nanocube electrode for the hydrogen evolution reaction (HER) was shifted to the positive direction (i.e., requiring a lower overpotential) by 20–40 mV compared to planar MoS2 films. This indicates that the nanocube electrodes have a significantly increased HER activity, which is probably because of a higher density of catalytically active edge sites available at the nanocube surface. It was also found that the HER activity initially increased with increasing MoS2 deposition time, but decreased after deposition for 60 min because the edges of the nanocubes became rounded, thereby decreasing the number of active edge sites. By depositing Ni and Pt on top of PMMA–Au nanocubes, it was shown that this method can also be used for the synthesis of nanocube structures with varying compositions.