High-index Bi2Se3(221) film has been grown on In2Se3-buffered GaAs(001), in which a much retarded strain relaxation dynamics is recorded. The slow strain-relaxation process of in epitaxial Bi2Se3(221) can be attributed to the layered structure of Bi2Se3 crystal, where the epifilm grown along [221] is like a pile of weakly-coupled quintuple layer slabs stacked side-by-side on substrate. Finally, we reveal strong chemical bonding at the interface of Bi2Se3 and In2Se3 by plotting differential charge contour calculated by first-principle method. This study points to the feasibility of achieving strained Tls for manipulating the properties of topological systems. (C) 2016 Elsevier B.V. All rights reserved.