Due to the extreme rise of sludge pollution with heavy metals (e.g. copper), the options for its disposal or treatment are decreasing. On the contrary, properly heavy metal-cleaned sludge can be used as an alternative sustainable energy and agriculture source. The aim of this study was to develop a novel nanoadsorbent, based on irreversibly linked amino-rich polymer onto previously silica-coated magnetic nanoparticles (MNPs) that can be applied efficiently for metal removal. MNPs were coated uniformly by 3 nm thick silica layer (core-shell structure), and were additionally modified with systematic covalent attachment of derived branched polyethyleneimine (bPEI). The formed structure of synthesized MNPs composite was confirmed with several analytical techniques. Importantly, nanoadsorbents exhibit high density of chelating amino groups and large magnetic force for easier separation. The importance of introduced bPEI, effect of pH, initial heavy metal concentration onto copper uptake efficiency and, further, nanoadsorbent regeneration, were studied and explained in detail. The adsorption isotherm was well fitted with Langmuir model, and the maximum adsorption capacity was shown to be 143 mg·g1 for Cu2+. The reusability and superior properties of silica-coated MNPs functionalized with derived-bPEI for copper adsorption underlie its potential for the removal application from heavy metals contaminated sludge.