In article number 1801233, Ramanathan Vaidhyanathan and co-workers show that ordered porosity with aligned functional groups in a covalent organic framework provide confinement for the growth of small-sized ferromagnetic cobalt nanoparticles. This composite nanocatalyst shows exceptional activity for H2 evolution from cheap and readily available NaBH4. This heterogeneous catalyst offers chemoselective products in one pot reduction reactions under aqueous and harsh basic/acidic conditions, with an activity comparable to noble metal (Au, Pd, Pt) based catalysts.