Nigeria is undergoing a major transition in its transportation and energy sectors, driven by fuel subsidy removal, rising costs, and the government’s push for low-carbon mobility through the Presidential Compressed Natural Gas Initiative (PCNGI). This study assesses national readiness and pathways for accelerating the adoption of Compressed Natural Gas (CNG) as a viable bridge fuel toward Nigeria’s Net-Zero 2060 targets. Anchored theoretically in the Technological Innovation Systems (TIS) framework, this study employed a cross-sectional perception survey design over a three-month period. Data was gathered from a purposively selected sample of 110 elite stakeholder group respondents across key operational sectors—including government, transport, and energy—spanning all six geopolitical zones, with a primary concentration in the South-West and North-Central regions. The findings demonstrate an extremely high level of CNG awareness (98%) and robust positive sentiment regarding its economic, environmental, and public-health benefits. However, actual adoption remains severely restricted by deep structural barriers. The primary constraints identified by respondents include insufficient refueling stations (74%), prohibitive vehicle conversion costs (68%), and a lack of flexible financing options. These challenges highlight critical systemic weaknesses in resource mobilization and market formation within the TIS framework. To convert strong latent demand into widespread uptake, a coordinated national strategy is required. The study recommends strategic imperatives including a Public–Private Partnership (PPP) model, robust investment in refueling infrastructure, targeted conversion subsidies, localized manufacturing of CNG components, and enhanced regulatory safety standards to establish a sustainable CNG market ecosystem.