We report on an innovative approach to fabricate lithium ion battery anodes based on optimized growth of hybrid carbon nanotube (CNT) and graphene nanostructures directly on copper foil substrates by an ambient pressure chemical vapor deposition process. Seamlessly connected graphene and CNT pillars provide a relatively strong active material-current collector integrity, which facilitates charge transfer in the system. This innovative architecture provides a binder-free technique for preparing electrodes for lithium ion batteries.