2D/1D-MoS2/TiO2 heterostructures have proven to be vigorous for photocatalytic applications. The enhancement in photocatalytic activity of heterostructures may get influenced by the accumulation of strain at the interface that affects the interfacial interaction. Keeping that in view, present paper reports the strain accumulated interfacial modification of 2D/1D-MoS2/TiO2 heterostructures for the enhancement of photocatalytic activity. Two different synthesis methods such as hydrothermal and chemical vapour deposition (CVD) method are used for the growth of MoS2 on TiO2 nanostructures. Micro-Raman spectroscopy revealed that strain is accumulated at the interface on growth of MoS2 over TiO2 nanostructures. It is further revealed that the MoS2/TiO2 heterostructure synthesized by CVD method induces compressive strain. Also, heterostructures synthesize by hydrothermal method induces tensile strain that modify the charge separation at the interface, which was further confirmed by X-ray photoelectron spectroscopy (XPS). Moreover, ultraviolet photoelectron spectroscopy (UPS) revealed that the upward band bending in the MoS2/TiO2 heterostructures synthesized by hydrothermal method. Similarly, heterostructure synthesized by chemical vapour method (CVD) shows the downward band bending that leads to the improved charge separation at interface. The modified interface of heterostructures is further studied for electrochemical measurement using cyclic voltammetry (CV) and photocatalytic activity by degradation of model compound.