Co-optimization of the gallium and sulfur profiles in penternary Cu(In,Ga)(Se,S)2 thin film solar cell and its impacts on device performance and variability are investigated in this work. An absorber formation method to modulate the gallium profiling under low sulfur-incorporation is disclosed, which solves the problem of Ga-segregation in selenization. Flatter Ga-profiles, which lack of experimental investigations to date, are explored and an optimal Ga-profile achieving 17.1% conversion efficiency on a 30 cm × 30 cm sub-module without anti-reflection coating is presented. Flatter Ga-profile gives rise to the higher Voc × Jsc by improved bandgap matching to solar spectrum, which is hard to be achieved by the case of Ga-accumulation. However, voltage-induced carrier collection loss is found, as evident from the measured voltage-dependent photocurrent characteristics based on a small-signal circuit model. The simulation results reveal that the loss is attributed to the synergistic effect of the detrimental gallium and sulfur gradients, which can deteriorate the carrier collection especially in quasi-neutral region (QNR). Furthermore, the underlying physics is presented, and it provides a clear physical picture to the empirical trends of device performance, I-V characteristics, and voltage-dependent photocurrent, which cannot be explained by the standard solar circuit model. The parameter "FGa" and front sulfur-gradient are found to play critical roles on the trade-off between space charge region (SCR) recombination and QNR carrier collection. The co-optimized gallium and sulfur gradients are investigated, and the corresponding process modification for further efficiency-enhancement is proposed. In addition, the performance impact of sulfur-gradient variation is studied, and a gallium design for suppressing the sulfur-induced variability is proposed. Device performances of varied Ga-profiles with front sulfur-gradients are simulated based on a compact device model. Finally, an exploratory path toward 20% high-efficiency Ga-profile with robustness against sulfur-induced performance variability is presented.