Two-dimensional covalent organic frameworks (2D-COFs) are a class of crystalline porous organic polymers, consisting of 2D-planar sheets stacked together perpendicularly via noncovalent forces. Since their discovery, 2D-COFs have attracted extensive attention for optoelectronic and adsorption applications. Owing to the layer stacking nature of 2D COFs, various new slipped structures that are energetically favourable can be designed. These interlayer slipped structures are actively responsible for tuning (mostly enhancing) the optoelectronic properties, thermal properties, and mechanical strength of 2D COFs. This review summarizes the effect of interlayer slipping on the energetic stability, electronic behaviour and gas adsorption properties of 2D layered COFs, which is explained through computational modelling simulations. Since computational modelling offers a deep insight into electronic behaviour at the atomic scale, which is potentially impossible through experimental techniques, the introduction and role of computational techniques in such studies have also been described.