Photonic nanomaterials have contributed greatly to the development of photomedicines. However, the finite depth of light penetration is still a serious limitation. Here, we developed a poly(allylamine) (PAAm)-modified upconversion nanoparticle/hyaluronate−rose bengal (UCNP/PAAm/HA-RB) complex for photochemical bonding of deep tissue with NIR light illumination. Compared to the conventional invasive treatment, the UCNP/PAAm/HA-RB complex could be noninvasively delivered into the deep tissue and accelerate the tissue bonding upon NIR light. The NIR light triggered UCNP in the complex to illuminate green light under the skin tissue. The activated RB in the HA-RB conjugate by the green light induced radical formation for the crosslinking of incised collagen matrix. In vitro light propagation test, collagen fibrillogenesis analysis, in vivo animal tissue bonding test, and ex vivo tensile strength test confirmed the successful photochemical tissue bonding effect of UCNP/PAAm/HA-RB complex.