Use of long period gratings (LPGs) formed in grapefruit photonic crystal fiber (PCF) with thin-film overlay coated on the inner surface of air holes for gas sensing is demonstrated. The finite-element method was used to numerically simulate the grapefruit PCF–LPG modal coupling characteristics and resonance spectral response with respect to the refractive index of thin-film inside the holey region. A gas analyte-induced index variation of the thin-film immobilized on the inner surface of the holey region of the fiber can be observed by a shift of the resonance wavelength. As an example, we demonstrate a 2,4-dinitrotoluene (DNT) sensor using grapefruit PCF–LPGs. The sensor exhibits a wavelength blue-shift of ∼820 pm as a result of exposure to DNT vapor with a vapor pressure of 411 ppbvat 25°C, and a sensitivity of 2 pm ppbv−1 can be achieved.