The mixing morphology control plays a crucial role in photovoltaic power generation,yet this specific effect on device performances remains elusive.Here,we employed computational approaches to delineate the photovoltaic properties of layered heterojunction polymer solar cells with tunable mixing morphologies.One-step quench and two-step quench strategies were proposed to adjust the mixing morphology by thermodynamic and kinetic effects.The computation for the one-step quench revealed that modulating interfacial widths and interfacial roughness could significantly promote the photovoltaic performance of layered heterojunction polymer solar cells.The two-step quench can provide a buffer at a lower temperature before the kinetic quenching,leading to the formation of small-length-scale islands connected to the interface and a further increase in photovoltaic performance.Our discoveries are supported by recent experimental evidence and are anticipated to guide the design of photovoltaic materials with optimal performance.