Refractive index (RI) sensing is a promising technique in a variety of different scientific and industrial applications. In this paper, we theoretically and experimentally propose a newly-designed RI sensor. The proposed sensor consists of a particular long-period fiber grating inscribed in a two-mode fiber (LPFG-TMF) coated with tunable graphene oxide (GO), and the special structure allows an extremely high sensitivity in the transition region. The mode coupling between the LP 11 core mode and the sixth-order cladding mode in the LPFG-TMF offers an apparently higher sensitivity feature. And the sensitivity is higher than that of a single-mode fiber-based LPFG (LPFG-SMF), which originates from the coupling between the core mode and the sixth-order cladding mode. Furthermore, the ultrasonic treatment time of GO, which impacts on the properties and performance of RI sensing, is also studied and investigated. Proof-of-concept results demonstrate significantly that comparing with the bare LPFG-TMF (621.66 nm/RIU) and LPFG-SMF coated with GO ultrasonicated 5 hours (323.68nm/RIU), the LPFG-TMF coated with GO ultra-sonicated 5 hours performs optimized sensitivity of 11605.79 nm/RIU when surrounding RI ranges from 1.4558 to 1.4577. With its premium ability to operate highsensitivity measurements, the RI sensing is expected to be useful for broad applications across the chemical fields. INDEX TERMS graphene oxide, long-period fiber grating, refractive index measurement, two-mode fiber.