Taking the dual-sublayer BiCuSeO superlattice thermoelectric material as an object, equivalent mono- and dual-doped samples were prepared by substitution of Bi and Cu atoms in the corresponding [Bi₂O₂]²⁺ sublayer and [Cu₂Se₂]^2- sublayer with isovalent La and Ag atoms. Their thermoelectric properties and the defect modulation mechanism were studied. The results showed that La-Ag dual-doped sample could combine the advantages of mono-doped samples to achieve an relative high carrier mobility while moderately increasing the carrier concentration, thereby maximizing the electrical conductivity. At the same time, it can also induce a potential band convergenceeffect, achieving the low average band effective mass and high density of states effective mass at the same time, which finally endowed Bi_0.98La_0.02Cu_0.98Ag_0.02SeO with simultaneous high carrier mobility and Seebeck coefficient, as well as the optimized power factor (PF=σS²). On the other hand, due to the strong point defect scattering on the heat-carrying phonons, the lattice and total thermal conductivities of these isovalent doped samples were further reduced, which finally optimized the figure of merit (ZT). As a result, a high ZT value of 0.46 was achieved at 755K in the La-Ag dual-doped sample, which was superior to that of the pristine sample (0.27 at 755 K) as well as the mono-doped counterparts. Present work demonstrates that heterolayer-isovalent dual-doping with La/Ag equivalent atoms in BiCuSeO can synergistically modulate its thermoelectric transport parameters with significantly improved thermoelectric performance.