A strategy for the synthesis at room temperature of binderless 3D sphere-like aggregates of bimetallic PtRh nanoparticles onto carbon nanotubes (CNTs) by cross-beam laser deposition technique is presented. The atomic ratio between the two components (Pt and Rh) is tuned by varying the laser pulse energy on the two targets independently to optimize the alloying effects. The morphology of PtRh alloy nanostructure is controlled by introducing helium gas under 2 Ton of pressure during growth. The prepared CNT/D-3 sphere-like aggregates bimetallic PtRh nanostructures provide a high degree of electrochemical activity and good durability toward the ethanol oxidation reaction (EOR) outperforming CNT/Pt and CNT/Pt3Sn, which is the most actively known electrocatalyst for EOR. Therefore, the 3D CNT/PtRh alloy porous nano structures provide a good prospect to explore their catalytic properties for direct ethanol fuel cells systems. (C) 2017 The Electrochemical Society. All rights reserved.