We report on the synthesis, structural, DC magnetic susceptibility studies on Gd2(MoO4)3 and Tb2(MoO4)3 polycrystals, prepared by conventional solid-state reaction method. Temperature and magnetic field (H) dependent magnetization and heat capacity measurements have been carried out to estimate the isothermal magnetic-entropy change (−ΔSm) and adiabatic temperature change (ΔTadi) in both rare-earth molybdates. No obvious long-range magnetic ordering can be found down to 2 K in both studied compounds. The estimated maximum value of –ΔSm at 3.5 K for 70 kOe is 31.1 J kg−1 K−1 and 16.7 J kg−1 K−1 in Gd2(MoO4)3 and Tb2(MoO4)3, respectively. Further, the calculated total-adiabatic temperature change for Gd2(MoO4)3 was 12.8 K, and Tb2(MoO4)3 has shown 9.8 K. The difference in the observed magnetocaloric and adiabatic temperature responses of Tb2(MoO4)3 compared to Gd2(MoO4)3 could be attributed to the presence of orbital angular moment of Tb3+ ions and relatively low-value of magnetization. Both the systems show a large magnetocaloric effect (MCE) (−ΔSm ∼ 12 J kg−1 K−1) even in low applied H (<20 kOe) attainable by a permanent magnet. Large magnetocaloric behaviour of Gd2(MoO4)3 and Tb2(MoO4)3 systems at a moderate field change along with very low electrical conductivity and the absence of thermal and magnetic field hysteresis in magnetization make them conducive to their use as promising magnetic refrigerants in the vicinity of liquid-helium temperatures.