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The synthesis, characterization, and incorporation of open-cage [60]fullerene derivatives as electron-transporting materials (ETMs) in perovskite solar cells (PSCs) with an inverted planar (p-i-n) structure is reported. Following optical and electrochemical characterization of the open-cage fullerenes <b>2a</b>&#8211;<b>c</b>, p-i-n PSCs with a indium tin oxide (ITO)/poly(3,4-ethylenedioxythiophene)-polystyrene sulfonate (PEDOT:PSS)/perovskite/fullerene/Ag structure were prepared. The devices obtained from <b>2a</b>&#8211;<b>b</b> exhibit competitive power conversion efficiencies (PCEs) and improved open-circuit voltage (<i>V_oc</i>) values (&gt;1.0 V) in comparison to a reference cell based on phenyl-C₆₁-butyric-acid methyl-ester (PC₆₁BM). These results are rationalized in terms of a) the higher passivation ability of the open-cage fullerenes with respect to the other fullerenes, and b) a good overlap between the highest occupied molecular orbital/lowest unoccupied molecular orbital (HOMO/LUMO) levels of <b>2a</b>&#8211;<b>b</b> and the conduction band of the perovskite.