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The encapsulation of small non-noble metal nanoparticles (NPs) within an inorganic layer has received considerable attention owing to their enhanced stability and high catalytic activity. Using a combination of emulsion-free polymerization, inner RF-Ni2+ and outer SiO2 coating, and subsequent carbonization treatment, herein, we have fabricated worm-like structured Ni-based composites in which a high density of nickel NPs are embedded in a carbon layer and also entrapped by SiO2 nanocages. We find that the carbonization temperature plays a vital role in adjusting the size of the Ni NPs. A detailed examination of the encapsulated nickel particles synthesized at 700 °C exhibited the best performance on the catalysis of the reduction of 4-NPs. Moreover, owing to the good alloying ability of the Ni NPs with noble metal NPs, the Ni-Pd alloy NPs are also entrapped in the SiO2 nanocages, which exhibit better performance on the catalysis than the Ni-based composites. The encapsulation of Ni-Pd alloys within SiO2 nanocages also improves stability against agglomeration and metal separation during catalytic operation.