Atomic layer deposition (ALD) is a facile process to decorate carbon surfaces with redox-active nanolayers. This is a particularly attractive route to obtain hybrid electrode materials for high performance electrochemical energy storage applications. Using activated carbon and carbon onions as representatives of substrate materials with large internal or external surface area, we have studied the enhanced energy storage capacity of vanadium oxide coatings. While the internal porosity of activated carbon readily becomes blocked by obstructing nanopores, carbon onions enable the continued deposition of vanadia within their large interparticle voids. Electrochemical benchmarking in lithium perchlorate in acetonitrile (1 M LiClO4) showed a maximum capacity of 122 mAh/g when using vanadia coated activated carbon and 129 mAh/g for vanadia coated carbon onions. There is an optimum amount of vanadia between 50-65 wt.% for both substrates that results in an ideal balance between redox-activity and electrical conductivity of the hybrid electrode. The stability of both systems is promising, with a capacity retention of ~95 % after 3,000 cycles. Assembling asymmetric (charge balanced) full cells, a maximum specific energy of 38 Wh/kg and 29 Wh/kg was found for the system employing carbon onions or activated carbon, respectively.