Extensive research efforts are currently devoted to alternative materials for photovoltaic (PV) applications that can overcome issues of the currently dominating thin film solar cell technologies, namely, such as CdTe and Cu(In, Ga)Se2 (CIGS). In this context, the kesterite compound Cu2ZnSn(S,Se)4 (CZTS) containing earth-abundant and non-toxic elements, as well as an optimal direct bandgap at 1.5 eV, is a promising candidate for PV applications. However, the efficiency of CZTSSe of 12.6% achieved today is still below the ultimate goal of >20% efficiency. In particular, the synthesis of CZTS is rather challenging due to its relatively narrow phase region and good control of the composition is critical for obtaining high performance solar cells. In this paper, we will discuss the synthesis of the quaternary CZTS compound by pulsed laser deposition (PLD). We will present different approaches for the deposition of CZTS: 1) room-temperature deposition followed by post-annealing and 2) growth of CZTS at high temperature. In the former approach, a sulfur evaporation beam assisting the deposition of CZTS is used to compensate for the sulfur loss. Our findings reveal that during ablation of a multicomponent CZTS target, the stoichiometry of the films can vary dramatically from a fluence from 0.2 J/cm2 to 2 J/cm2. In particular, films deposited at a low fluence of 0.2 J/cm2 are Cu-free, and the Cu content in the films increases monotonically with increasing fluence. Interestingly, this effect is less pronounced for ablation of a single-phase CZTS target.