Provided are methods of producing hollow metal nanospheres (HMNs) having a pre-selected surface rugosity. The methods include combining in a galvanic exchange reaction at a selected pH: a solution comprising cobalt-based nanoparticle (CoxBy NP) scaffolds; and a solution comprising a metal, to produce CoxBy NP core/metal shell structures. The methods further include oxidizing the CoxBy NP cores of the CoxBy NP core/metal shell structures to produce HMNs having the pre-selected surface rugosity, where the pH of the galvanic exchange reaction is selected to produce the pre-selected surface rugosity of the HMNs. Also provided are HMNs produced according to the methods, as well as methods of using the HMNs. Compositions and kits that find use, e.g., in practicing the methods of the present disclosure, are also provided.