Epoxy resin (EP) is quite flammable, which limits its application in areas such as coatings and electronic and electrical materials. In this study, 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO) (or diphenylphosphine oxide (DPO)) 3-cyclohexene-1-formaldehyde (CC) and 4,4’diaminodiphenylmethane (DDM) were selected for the synthesis of two rich aromatic and phosphorus-containing compounds (DOPO-CC and DPO-CC). DOPO-CC and DPO-CC were introduced into epoxy pre-polymers to prepare epoxy thermosets with flame retardancy. When 5 wt% DOPO-CC (P content of 0.50 wt%) or DPO-CC (P content of 0.52 wt%) was added, the LOI values of the epoxy thermosets increased from 25.5% (pure EP) to 33.5% (EP added DOPO-CC) and 31.0% (EP added DPO-CC), respectively, and these epoxy thermosets also achieved the UL-94 V-0 rating. Additionally, cone calorimeter tests showed that the peak heat release rate (PHRR) and total heat release (THR) of epoxy thermoset containing 5 wt% DPO-CC reduced by 42.0% and 39.7% compared to those of pure EP, respectively. By reducing the thermal degradation rate (condensed phase) and combining and quenching free radicals (gaseous phase), the introduction of DOPO-CC or DPO-CC can efficiently improve the flame retardancy of epoxy thermosets. More importantly, the epoxy thermosets containing DOPO-CC or DPO-CC exhibited better mechanical properties than pure EP, which could be proven by the storage modulus and tensile strength. This study provided a new class of rich aromatic and phosphorus-containing compounds that can serve as co-curing agents for epoxy thermosets with outstanding comprehensive performances.