Silicon can play a central role in the next generation Li-ion batteries. Certainly, silicon’s advantages, namely its exceptional specific capacity and low working voltage, are overshadowed by the associated instabilities: lithiation-induced stresses that can generate material degradation and solid electrolyte interface damage. Despite the plethora of engineered nanostructures developed to address these vulnerabilities, commercial adoption of Si-based anodes requires low-cost, scalable and simple manufacturing processes. Here, we report on three-dimensionally interconnected Si-based aerogel systems based on silicon nanostructures trapped within highly porous, electronically active multi-walled carbon nanotube (MWCNT) frameworks as lithium-ion battery anodes. For the homogeneity of the anode composite, Si is modified with polyaniline. The genuine Si-MWCNTs blend is enabled by polyaniline through π- π interactions in butanol. Next, butanol gelation is achieved by ultra-slow filtration with a Millipore system; this results in a unique Si-MWCNTs framework suspended in a butanol gel. Finally, critical point drying is used to evaporate the solvent and to maintain the integrity of the Si-MWCNTs porous framework. This Si-based aerogel configuration offers several advantages compared with the traditional slurry-coated electrodes. The observed electrochemical features are promising; we attribute them to the aerogel structure that supports a high strain allowing for Si expansion/contraction and ensures the electrolyte flow. For example, the Si-based aerogels were electrochemically evaluated in half-cell configurations and exhibit stable cycling even at high current densities rates. This simple method for the preparation of aerogels is valuable for other active materials available for the Li-ion energy storage technology that show volume variation during Li shuttling.