Significance The rapid development of flexible and portable electrochemical energy devices has promoted the demand for flexible and lightweight electrocatalysts. Here we report flexible high performance electrocatalysts based on PtCu alloy nanotube arrays on carbon fiber cloth (CFC) (PtCu ANTAs/CFC) for direct methanol fuel cell (DMFC). Compared with Pt NTAs/CFC and commercial Pt/C, the PtCu ANTAs/CFC electrocatalysts exhibit significantly improved electrocatalytic activity and durability. Furthermore, the PtCu ANTAs/CFC electrocatalysts show excellent flexibility and they can keep almost constant electrocatalytic performance under the different distorted states, such as normal, bending and twisting states. The improved performance of the flexible PtCu ANTAs/CFC electrocatalysts can be ascribed to unique ANTAs, synergistic effect between Pt and Cu, and porous structure of CFC. This work shows the significant progress of high-performance Pt-based flexible anodes for DMFCs. (c) 2016 American Institute of Chemical Engineers AIChE J, 62: 975-983, 2016