One of the exciting applications of electron-spin-based quantum sensing is the detection of distant nuclear spins of external molecular species. Here, we explore the application of a metal-organic framework (MOF) material as a host matrix for sensing spin centers. As a sensor, we employ inherent Cu2+ ions in the structure of a Zn-doped HKUST-1 framework. As a target molecular species, we use butane gas that exhibits no specific chemical reactivity toward the inner surface of HKUST-1 and is thus randomly distributed inside the MOF pore network. By employing a conventional double-resonance pulse sequence, we can effectively detect the coupling of the distant 1H nuclear spins of butane to the electron spin of the sensor and gain atomic-scale insight into their spatial distribution. Thus, our proof-of-the-concept experiment demonstrates that MOFs, the materials featuring extremely large surface area and great tunability, are perfectly suited as a key element for emerging magnetic quantum sensing solutions.