Corneal defects are associated with corneal tissue engineering in terms of vision loss. The treatment of corneal defects is an important clinical challenge due to a uniform corneal thickness and the apparent lack of regenerative ability. In this work, we synthesized a biocompatible and photocrosslinkable ocular tissue adhesive composite hydrogel prepared by using methacrylated gelatin (GelMA), which is called the most favorable derivative of gelatin used as a tissue adhesive, silk fibroin (SF), and GelMA/SF (GS) with high adhesion behaviours for use in corneal injuries. The adhesion behaviours of the materials prepared in the presence of silk fibroin were improved. Importantly, the effect of different UV curing times on the adhesion properties of the prepared materials was also investigated. The prepared GS tissue adhesives showed high physiological adhesion. GS can be modulated to increase its adhesive strength up to 3 times compared to G. GS was also found to be biocompatible and have a high healing potential. In addition, the obtained transmission value of GS is also close to that of the human cornea. GS supported cellular adhesion and proliferation. The burst pressure strength for fresh cornea of the GS-60s sealants (144.5 ± 13 kPa) was determined to be higher than that of the G-60s sealants (52.6 ± 33.5 kPa).