Metal-salophen molecular chains are promising candidates for designing spintronic devices due to their magnetic coupling, thermal stability and self-assembly. Based on first principles calculations, we systematically investigate the energetic, electronic, magnetic, and spin-resolved transport properties of salophen-based molecular chains with various metal centers, i.e. X-salophen (X = Sc-Ni and Y-Mo). The results show that the X-salophen (X = Sc-Ni and Y-Mo) molecular chains have high energetic stability and synthetic feasibility. The magnetic moments of transition metal atoms at the molecular centers decrease by 0.87 μB–3.98 μB compared with the isolated atoms, as a result of electron rearrangement during forming coordinate bonds. The band structures exhibit a prominent spin polarization around Fermi level of X-salophen (X = Co, Cr, Fe and Mo) molecular chains. The devices based on these chains present excellent spin-polarized transport performance in the low bias range: X-salophen (X = Co, Cr, Fe and Mo) molecular devices with parallel spin configurations exhibit almost ideal spin filtering efficiency of 100% independent of the bias, and as for antiparallel spin cases, the devices show dual-direction spin-filtering effect; a giant magnetoresistance effect of 102 to 103 is found for Cr, Fe and Mo cases under low bias, and 109 for Co case in whole considered bias range. Our study provides a reference for designing high-performance spintronic devices based on metal-salophen molecular chains.