Two-dimensional (2D) materials have attracted increasing interest in the past decades due to their unique physical and chemical properties for diverse applications. In this work, we present a first-principles design on a novel 2D family, MSi2CxN4−x (M = Cr, Mo, and W; x = 1 and 2), based on density-functional theory (DFT). We find that all MSi2CxN4−x monolayers are stable by investigating their mechanic, dynamic, and thermodynamic properties. Interestingly, we see that the alignment of magnetic moments can be tuned to achieve non-magnetism (NM), ferromagnetism (FM), anti-ferromagnetism (AFM) or paramagnetism (PM) by arranging the positions of carbon atoms in the 2D systems. Accordingly, their electronic properties can be controlled to obtain semiconductor, half-metal, or metal. The FM states in half-metallic 2D systems are contributed to the hole-mediated double exchange, while the AFM states are induced by super-exchange. Our findings show that the physical properties of 2D systems can be tuned by compositional and structural engineering, especially the layer of C atoms, which may provide guidance on the design and fabrication of novel 2D materials with projected properties for multi-functional applications.