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Aluminum scandium nitride (AlScN) has attracted extensive attention for its excellent piezoelectric properties in the micro‐electromechanical system applications. In this work, AlScN is demonstrated to be a promising candidate for on‐chip acousto‐optic coupling interactions with outstanding piezoelectric properties as well. Based on piezoelectric Al_0.6Sc_0.4N film deposited on silicon‐on‐insulator platform, the proposed devices exhibit impressive acousto‐optic coupling performances over a short interaction length of 210 µm with surface acoustic waves actuated by interdigital transducers. Meanwhile, the acousto‐optic coupling performances are further improved in a compact spiral waveguide with eight interaction segments, where the measured modulation efficiency is enhanced from −21.5 to −12.5 dB and the radiofrequency (RF) 3‐dB bandwidth is narrowed from 4 to 3.1 MHz at central frequency of 3.044 GHz …