To develop a multipurpose dental adhesive resin, the effects of polymerization initiator systems comprising ti-monosubstituted barbituric acid (5-MSBA), aromatic sulfinate amide (ASA), and tert-butyl peroxymaleic acid (t-BPMA) with 4-acryloxyethyltrimellitic acid (4-AET) or its anhydride (4-AETA) on adhesion and curing time were investigated. Tensile bond strength values of a Ni-Cr alloy are affected by the inclusion of t-BPMA, and the optimum concentration of t-BPMA in a 5-MSBA-ASA-t-BPMA-type initiator system was found to be 0.5-2.0 wt %, and it was noteworthy that the correlation between the tensile bond strength and curing time on the t-BPMA-concentration showed a highly negative correlation of a benzenesulfinate morphoride (BSMo) series adhesive: r = -0.957, and a p-toluenesulfinate morphoride (p-TSMo) series adhesive: r = -0.949. The combination of 1-cyclohexyl-5-ethylbarbiturioc acid (CEBA) with ASA provides a high level of tensile bond strength to the Ni-Cr alloy, and the optimum concentration of CEBA in a CEBA-ASA-t-BPMA-type initiator and the bond strength values were found to be 0.75 wt % CEBA: 52.3 MPa (with BSMo), and 1.0 wt % CEBA: 50.9 MPa (with p-TSMo), respectively. It was suggested that 5-MSBA, ASA, and t-BPMA and their combinations provided the environment where 4-AETA exhibited good bonding performance with increasing wettability to metal without interference of a charge-transfer complex derived from a polymerization initiator system such as benzoyl peroxide (BPO)-amine.