This paper presents the fabrication and application of a notched long-period fiber grating (NLPFG) with an amine-modified surface nanostructure for carbon dioxide (CO2) gas sensing. The NLPFG with the modified surface nanostructure was fabricated by using inductively coupled plasma (ICP) etching with an Ag nanoparticle etching barrier. The experimental results show that the spectra were changed with the CO2 gas flow within 12 min. Thereafter, the spectra of the NLPFG remained steady and unchanged. During the absorption process, the transmission loss was decreased by approximately 2.019 dB, and the decreased rate of transmission loss was 0.163 dB/min. The sensitivity was about −0.089 dB/%. These results demonstrate that the NLPFG CO2 gas sensor has the advantages of steady performance, repeatability, and low cost. Therefore, the NLPFG can be utilized as a reliable CO2 gas sensor.