Silicon is emerging as a very attractive anode material for lithium ion batteries due to its low discharge potential, natural abundance, and high theoretical capacity of 4200 mAh/g, more than ten times that of graphite (372 mAh/g). This high charge capacity is the result of silicon’s ability to incorporate 4.4 lithium atoms per silicon atom; however, the incorporation of lithium also leads to a 300-400% volume expansion during charging, which can cause pulverization of the material and loss of access to the silicon. The architecture of the anode must therefore be able to adapt to this volume increase. Here we present a layered carbon nanotube and silicon nanoparticle electrode structure, fabricated using directed assembly techniques. The porous carbon nanotube layers maintain electrical connectivity through the active material and increase the surface area of the current collector. Using this architecture, we obtain an initial capacity in excess of 4000 mAh/g, as well as increased power and energy density as compared to anodes fabricated using the standard procedure of slurry casting.