In this study, FeCoNi alloy nanoparticles were combined with Nd(OH)3 nanostructures to create unique cotton-like nanoparticles (C-NPs). These C-NPs were synthesized through an accessible, two-step reactive chemical milling process. The nanoparticles originated from a blend of metal chlorides (FeCl2, CoCl2, and NiCl2) and sodium (Na), used as a precursor in the reaction, within a SPEX milling apparatus. The Fe, Co, and Ni were maintained at equal weight percentages (1:1:1). Subsequently, NdCl3 and Na were utilized to facilitate the attachment of Nd(OH)3 nanostructures onto the FeCoNi nanoparticles through a solid-state reaction in the same SPEX milling setup. The Nd content was varied to investigate its effect on the integration of Nd(OH)3 onto the surface of CoNiFe nanoparticles. Electron microscopy revealed the formation of cotton-like nanoparticles, and the distribution of elements was identified using secondary ion mass spectrometry. The CoNiFe alloy and Nd(OH)3 phases were verified by X-ray diffraction analysis. These nanoparticles were internalized into cells via endocytosis, as observed in transmission electron microscopy images after incubation with the BT20 cell line (triple-negative breast cancer), likely due to interactions between –OH groups and the cell membrane. Following this, the cells containing C-NPs underwent photoluminescence studies, revealing two distinct emission peaks at 400 nm, and 486 nm. X-ray photoelectron spectroscopy indicated the presence of various heterostructures within the FeCoNi-Nd(OH)3 complex, which may be responsible for these emission properties.