For highly efficient heat dissipation of thin electronic devices, development of film materials that exhibit high thermal conductivity in the in-plane direction is desired. In particular, it is important to develop thermally conductive films with large in-plane anisotropy to prevent thermal interference between heat sources in close proximity and to cool in other directions by diffusion. In this study, we developed flexible composite films composed of a uniaxially aligned carbon-fiber filler within a cellulose nanofiber matrix through liquid-phase three-dimensional patterning. The film exhibited a high in-plane thermal conductivity anisotropy of 433%, with combined properties of a thermal conductivity of 7.8 W/mK in the aligned direction and a thermal conductivity of 1.8 W/mK in the in-plane orthogonal direction. This remarkable thermal conductivity and in-plane anisotropy showed the ability to significantly cool powder electroluminescent devices formed on the composite film and also to cool two heat sources in close proximity without thermal interference. In addition, the carbon-fiber filler could be extracted from the composite films by heat treatment at 450 °C and reused as a thermally conductive material.