Molybdenum disulfide (MoS2) is a promising alternative to graphite anodes in battery materials. Therefore, it is critical to scrutinize their structural stability and charge storage capacity during battery operation. In this study, freestanding electrodes consisting of MoS2‐incorporated carbon nanotube aerogels (MSCA) were fabricated using a simple yet scalable hydrothermal method, as used in lithium‐ion batteries. The outer nitrogen‐doped graphitic carbon (NGr) layers support efficient charge transport, even under a substantial compressive environment, and improve the structural integrity, showing significant improvements in battery performance, such as a high rate capacity of 820 mAh g−1 at the current density of 5 A g−1 and 94% capacity retention after 170 cycles (1170 mAh g−1 at 1 A g−1 after 170 cycles), even in the absence of polymer binders and conductive additives. The resulting NGr/MoS2/Single‐Walled Carbon Nanotubes (SWCNT) freestanding electrodes have great potential to increase the volumetric and gravimetric energy density of batteries.This article is protected by copyright. All rights reserved.