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Summary: While photocatalytic technology has brought additional opportunities and possibilities for the green conversion and sustainable development of ammonium-based nitrogen fertilizers, the low activation efficiency of the molecular N2 has impeded its further application feasibility. Here to address the concern, we designed an amorphous molybdenum hydroxide anchored on the ultrathin magnesium-aluminum layered double hydroxide (Mo@MgAl-LDH) nanosheets for benefiting the N2 photofixation to NH3. With the aid of the designed amorphous Mo(V) species, the pristine MgAl-LDH exhibited a considerable performance of nitrogen photofixation under visible light irradiation (NH3 production rate of 114.4 μmol g−1 h−1) due to the improved N2 activation efficiency. The work demonstrated a feasible strategy for nitrogen photofixation using amorphous Mo(V) species, which may also deliver a novel inspiration for the development of amorphous photocatalysts toward the photoactivation of molecular N2.