In this paper, we mainly prove a congruence conjecture of Z.-W. Sun \cite{Sjnt}: Let $p>5$ be a prime. Then $$ \sum_{k=(p+1)/2}^{p-1}\frac{\binom{2k}k^2}{k16^k}\equiv-\frac{21}2H_{p-1}\pmod{p^4}, $$ where $H_n$ denotes the $n$-th harmonic number. Comment: 19 pages, this is a preliminary draft, comments are welcome. arXiv admin note: text overlap with arXiv:2201.03418