The hierarchical TiO2 (H-TiO2) nanorod arrays (NRAs) composed of single-crystalline nanorods and nanocrystals were finely designed and successfully constructed for electrochromic (EC) application. By combining layer-by-layer (LBL) method and hydrothermal crystallization technique, the superfine nanocrystals (5-7 nm), which can provide abundant active sites and facilitate ion insertion/extraction during EC reactions, were uniformly and conformally assembled on the surface of single-crystalline TiO2 (SC-TiO2) NRAs. The as-formed H-TiO2 NRAs integrate the advantages of one-dimensional NRAs with fast kinetics and superfine nanocrystals with high ion capacity, showing highly enhanced EC performance. Large optical contrast (40.3%), shorter coloring/bleaching time (22/4 s), high coloration efficiency (11.2 cm(2) C-1), and excellent cycling stability can be achieved in H-TiO2 NRAs, superior to the pristine SC-TiO2 NRAs and nanocrystalline TiO2 films. This work provides a feasible and well-designed strategy to explore high-performance materials for EC application. (C) 2018 Elsevier B.V. All rights reserved.