Hydrogel composites are water-swollen and three-dimensional materials that have been investigated for various biological applications, including controlled drug delivery and tissue engineering, owing to the similarity between their mechanical, electrical, and chemical properties with biological tissues. The hydrogel composites can provide a superior replication of living tissue compared to their single components. In this regard, Fe-BTC, Cu-BTC, and Zn-BTC MOFs were synthesized and modified with gallic acid (GA). The MOFs-based hydrogel composites (M-BTC-GA@PVA-CS) were finally fabricated by freezing-thawing the as-synthesized MOFs, gallic acid, chitosan, and poly(vinyl alcohol) mixture. The obtained hydrogels were characterized using techniques such as FTIR, XRD, UV-vis, SEM, EDS, and TEM. Additionally, their antibacterial activity against E. coli and S. aureus and biocompatibility were investigated. The results showed that the surface modification of M-BTC MOFs with GA improves the antibacterial performance of hydrogels and increases their biocompatibility and cell viability. Among the as-prepared M-BTC MOF-based composites, the Cu-BTC MOF-loaded hydrogels showed the highest antibacterial activity. In contrast, the lowest antibacterial effect was observed for the hydrogels with Fe-BTC MOFs. Furthermore, the H&E staining exhibited improved vascularization in Zn-BTC-GA@PVA-CS and Cu-BTC-GA@PVA-CS scaffolds compared to the Fe-BTC-GA@PVA-CS hydrogel. These MOFs-loaded hydrogels may be suitable for utilization in biological applications such as skin treatment, drug delivery, and cosmetics owing to their excellent antibacterial activity and low cytotoxicity.