We present a concept of binderless nanothin catalyst layers for low power sources applications such as micro-fuel cells. The catalyst layer (CL) consists of pure CNTs catalyst support fabricated using chemical vapor deposition technique and a catalyst deposited by the pulsed laser deposition method. The whole CL is fabricated onto an electrically conductive carbon paper substrate. Synthesis of various morphologies of the catalyst including well-spread nanoparticles (NPs), interconnected NPs, and columnar-organized NPs were studied for their electroactivity toward methanol electro-oxidation. Pt was chosen as a model catalyst for fundamental studies. The best performing Pt/CNT layer developed here is made of a CNTs layer having a thickness between 200 and 370 nm plus the Pt layer of 50 nm. Adding Nafion ionomer to our CLs was detrimental to the electrochemical performance. The approach of binderless nanothin catalyst layers has the potential to be considerably more powerful than binder-containing conventional CLs. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.102203jes] All rights reserved.