Auxetic materials with multifunctional properties are highly sought after for application in modern nano-devices. However, the majority of reported inorganic auxetic materials exhibit low negative Poisson's ratios (NPR), poor flexibility, and limited functionality. In this study, we employ density-functional-theory (DFT) first-principles simulations to design a series of two-dimensional (2D) metal-organic frameworks (MOFs) M2C4X4 (M = Cu, Ag, Au; X = O, S, NCN) that display intriguing auxetic behavior, superior flexibility and appropriate photocatalytic water-splitting properties. These M2C4X4 MOFs are assembled from carbon tetragon motifs and exist in both cis- and trans-isomer forms, with the NPR ranging from -0.17 to -0.90. Notably, trans-Cu2C4(NCN)4 exhibits a high NPR of -0.90, while cis-Cu2C4(NCN)4 achieves an NPR of -0.67. Both isomers demonstrate excellent flexibility, characterized by ultra-low Young's modulus and high fracture strengths. Furthermore, their direct band gaps, strong light-harvesting capabilities, and long excited-state lifetimes make them promising candidates for the photocatalytic oxygen evolution reaction in water. These results provide a viable strategy for the design and synthesis of novel optoelectronic multifunctional materials.