Understanding
the nonlinear response of light and materials is
crucial for fundamental physics and next-generation electronic devices.
In this work, we have investigated the second-order nonlinear bulk
photovoltaic (BPV) and bulk spin photovoltaic (BSPV) effects in the
piezoelectric binary materials T-IV-VI and T-V-V (IV = Ge, Sn; VI
= S, Se; and V = P, As, Sb, Bi). The independent nonzero conductivity
tensors of charge current are derived for these binaries through the
symmetry analysis, along with the mechanism for generating pure spin
current. These binaries, with their unique folded structure, exhibit
significant charge and spin currents under illumination. Furthermore,
we find that strain engineering can effectively modulate charge/spin
currents by influencing charge density distribution and built-in electric
field due to the piezoelectric effect. Our research suggests that
the piezoelectric binary materials possess enormous and tunable charge/spin
currents, underscoring their potential for applications in nonlinear
flexible optoelectronics and spintronics.