Semiconducting piezoelectric α-In2Se3 and 3R MoS2 have attracted tremendous attention due to their unique electronic properties.Artificial van der Waals(vdWs)hetero-structures constructed with α-In2Se3 and 3R MoS2 flakes have shown promising applications in optoelectronics and photocatal-ysis.Here,we present the first flexible α-In2Se3/3R MoS2 vdWs p-n heterojunction devices for photodetection from the visible to near infrared region.These heterojunction devices exhibit an ultrahigh photoresponsivity of 2.9×103 A W-1 and a substantial specific detectivity of 6.2×1010 Jones under a compressive strain of-0.26%.The photocurrent can be increased by 64% under a tensile strain of+0.35%,due to the heterojunction energy band modulation by piezoelectric polarization charges at the hetero-junction interface.This work demonstrates a feasible approach to enhancement of α-In2Se3/3R MoS2 photoelectric response through an appropriate mechanical stimulus.