Acetaminophen (AC) is one of the most common over-the-counter drugs, and its pollutant in groundwater has attracted more attention due to its serious risk to human health. Currently, the research on AC is mainly focused on its detection, but few are concerned about its removal. In this work, for the first time, nitrogen-doped Soulangeana sepals derived biochar/β-cyclodextrin-Metal-organic frameworks (N-SC/β-CD-MOFs) composite was proposed for the simultaneous efficient removal and detection of AC. N-SC/β-CD-MOFs combined the properties of host-guest recognition of β-CD-MOFs and porous structure, high porosity, and large surface area of N-SC. Their synergies endowed N-SC/β-CD-MOFs with a high adsorption capacity toward AC, which was up to 66.43 mg/g. The adsorption type of AC on the surface of N-SC/β-CD-MOFs conformed to the Langmuir adsorption model, and the study of the adsorption mechanism showed that AC adsorption on N-SC was mainly achieved through hydrogen bonding. In addition, the high conductivity, large specific surface area and abundant active sites of N-SC/β-CD-MOFs were of great significance to the high-performance detection of AC. Accordingly, the sensor prepared with N-SC/β-CD-MOFs presented a wide linear range (1.0–30.0 μM) and a low limit of detection of 0.3 nM (S/N = 3). These excellent performances demonstrate that N-SC/β-CD-MOFs could act as an efficient dual-functional material for the detection and removal of AC.