Halloysite is a 1:1 dioctahedral clay mineral that has been studied widely for applications in nanotechnology and as a mineral exploration guide for recognizing regolith-hosted heavy rare earth element (HREE) deposits. In Brazil, pegmatites from the state of Rio de Janeiro have been catalogued, but their potential to host halloysite deposits has never been studied. After a mineral exploration programme, one pegmatite with considerable halloysite contents and economic potential was discovered. This study reports the mineralogical and chemical characterization of the halloysite of this pegmatite and evaluates the possibility of clay-adsorbed HREE deposits, like that in the Zudong (China) regolith-hosted HREE deposit. Seven samples were collected in horizontal channels. Bulk samples and clay fractions (<2 μm) were analysed by quantitative mineral analysis (X-ray diffraction/Rietveld method), chemical analysis (major elements by X-ray fluorescence and Y, U, Th and rare earth elements by inductively coupled plasma mass spectrometry), scanning electron microscopy, Fourier-transform infrared spectroscopy, particle-size analysis, nitrogen physisorption and cation-exchange capacity. Mixed polygonal/cylindrical halloysite-7Å in concentrations between 6.3 and 35.4 wt.% in bulk samples and between 58.0 and 89.8 wt.% in the clay fractions were identified in the pegmatite. The clay fractions presented an average chemical composition of 45.46 wt.% SiO2, 36.10 wt.% Al2O3, 14.62 wt.% loss on ignition and 1.04 wt.% Fe2O3, as well as technological properties close to those observed in world-class halloysite deposits such as Dragon Mine (USA) and Matauri Bay (New Zealand). The clay minerals did not present significant HREE contents.