Lithium iron phosphate (LFP) is currently one of the main cathode materials used in lithium-ion batteries due to its safety, relatively low cost, and exceptional cycle life. To overcome its poor ionic and electrical conductivities, LFP is often nanostructured, and its surface is coated with conductive carbon (LFP/C). Here, we demonstrate a sol–gel based synthesis procedure that utilizes a block copolymer (BCP) as a templating agent and a homopolymer as an additional carbon source. The high-molecular-weight BCP produces self-assembled aggregates with the precursor-sol on the 10 nm scale, stabilizing the LFP structure during crystallization at high temperatures. This results in a LFP nanonetwork consisting of interconnected ∼10 nm-sized particles covered by a uniform carbon coating that displays a high rate performance and an excellent cycle life. Our “one-pot” method is facile and scalable for use in established battery production methodologies.