Structures of thin films bonded on thick substrates are abundant in biological systems and engineering applications. Mismatch strains due to expansion of the films or shrinkage of the substrates can induce various modes of surface instabilities such as wrinkling, creasing, period doubling, folding, ridging, and delamination. In many cases, the film–substrate structures are not flat but curved. While it is known that the surface instabilities can be controlled by film–substrate mechanical properties, adhesion and mismatch strain, effects of the structures’ curvature on multiple modes of instabilities have not been well understood. In this paper, we provide a systematic study on the formation of multimodal surface instabilities on film–substrate tubular structures with different curvatures through combined theoretical analysis and numerical simulation. We first introduce a method to quantitatively categorize various instability patterns by analyzing their wave frequencies using fast Fourier transform (FFT). We show that the curved film–substrate structures delay the critical mismatch strain for wrinkling when the system modulus ratio between the film and substrate is relatively large, compared with flat ones with otherwise the same properties. In addition, concave structures promote creasing and folding, and suppress ridging. On the contrary, convex structures promote ridging and suppress creasing and folding. A set of phase diagrams are calculated to guide future design and analysis of multimodal surface instabilities in curved structures.