A highly sensitive, reversible, and linear sensor, exhibiting excellent stability in response to temperature and humidity, has been successfully proposed and demonstrated for the first time. This sensor is achieved by wrapping a polyvinyl alcohol/graphene nanofiber film onto a chiral long-period fiber grating (CLPG), which is fabricated by periodically twisting single mode fiber. In the experiment, the CLPG sensor demonstrates a temperature sensitivity of 74 pm/°C, which is approximately twice as high as that of conventional fiber grating sensors. Note that, by wrapping the graphene nanofiber film on CLPG, the temperature sensitivity of the sensor is up to 115.23 pm/°C in the range of 30°C to 75°C. In addition, CLPG using for humidity sensing is first demonstrated. The humidity sensitivity measures −9.92 pm/%RH with linearity of 0.995 during a change from 40%RH to 80%RH. In comparison to other humidity sensors, the sensitivity of the CLPG is comparable, whereas its sensing linearity stands out notably above the rest. The results show that CLPG has the characteristics of simple fabrication, easy combination with materials, stable performance, and high sensitivity and holds significant development potential in optical fiber sensing application fields.