Efficient insulation technology is one of the key technologies for the development of large LH2 storage tanks. This paper aimed at a 4000 m3 LH2 spherical tank, many insulation schemes were designed, including multilayer insulation systems integrated with a vapor-cooled shield (VCS) and liquid-nitrogen-cooled shield (LN2CS). The heat transfer model was developed to predict the insulation performance of a LH2 spherical tank. The effect of the VCS position on insulation performance was studied, and the different configurations of double VCSs were compared and discussed. The results showed that the daily evaporation rate of MLI, hollow glass microspheres (HGMs) and vacuum was only 2.05 × 10−3%, 3.62 × 10−3% and 7.94 × 10−2% at 1.34 Pa, respectively. MLI was still the optimal insulation scheme for a 4000 m3 LH2 spherical tank. Meanwhile, it was found that when the single VCS was placed at the 10th layer, the heat leakage was reduced by approximately 40.5% compared with MLI. The heat leakage of parallel VCS(P-VCS) was 76.6% lower than that of MLI. The minimum heat leakage of series VCS(S-VCS) was 83.79%, 72.75% and 37.36% lower than that of MLI, single VCS and P-VCS, respectively. Additionally, the heat leakage of the LH2 tank could be reduced to less than 10 W when LN2CS was installed. These results provide a design reference for the highly efficient storage of large LH2 tanks.