Concerning the trade-off between convergence and diversity in solving the multi-trip pickup and delivery Vehicle Routing Problem (VRP), a hybrid Non-dominated Sorting Genetic Algorithm Ⅱ (NSGA-Ⅱ) combining Adaptive Large Neighborhood Search (ALNS) algorithm and Adaptive Neighborhood Selection (ANS), called NSGA-Ⅱ-ALNS-ANS, was proposed. Firstly, considering the influence of the initial population on the convergence speed of the algorithm, an improved regret insertion method was employed to obtain high-quality initial population. Secondly, to improve global and local search capabilities of the algorithm, various destroy-repair operators and neighborhood structures were designed, according to the characteristics of the pickup and delivery problem. Finally, a Best Fit Decreasing (BFD) algorithm based on random sampling and an efficient feasible solution evaluation criterion were proposed to generate vehicle routing schemes. The simulation experiments were conducted on public benchmark instances of different scales, in the comparison experiments with the MA (Memetic Algorithm), the optimal solution quality of the proposed algorithm increased by 27%. The experimental results show that the proposed algorithm can rapidly generate high-quality vehicle routing schemes that satisfy multiple constraints, and outperform the existing algorithms in terms of both convergence and diversity.