Vertically aligned nanocomposite (VAN) thin film has attracted tremendous research interests owing to its multifunctionality, enhanced physical properties and multi-field coupling. However, VAN has rarely been demonstrated in flexible form, which hinders its further application in flexible devices. In this work, La0.67Sr0.33MnO3-CeO2 (LC) VAN film has been deposited on flexible mica with or without a buffer layer. The LC nanocomposite films show high quality following textured growth and form a typical, vertically aligned nanostructure. Magnetic, transport and magnetoresistance properties have been explored for flexible nanocomposite thin films. Furthermore, flexible LC films maintain their properties after numerous mechanical bending tests, presenting promising future applications in flexible electronics and spintronics.