Multiple catalytic active centers tactically generated on the 2-dimentional catalytic carrier could afford certain promoting function thanks to their existed special synergy. Herein, Ni-based nanosheet-like metasilicate catalytic materials were developed as heterogeneous catalysts towards styrene oxidation for the first time. Concurrently, the special heteroatom cobalt or magnesium-incorporated Ni-based nanosheet-like metasilicate were developed together via the proposed synthesis tactics. The resulted sheet-like nanomaterials were meticulously characterized and identified through valid techniques. The introduction of heteroatom metal elements of cobalt or magnesium incorporated in the Ni-based nanosheet-like metasilicate was proven to trigger the regulated catalytic effect including positive and negative aspects towards styrene oxidation, and their function was identified and understood based on the reaction exploration results, in which the present cobalt significantly give rise to the promotive catalytic conversion activity and selectivity towards styreneoxide(conversion 96.8%, selectivity 78.4%), while the magnesium oppositely induced the restraining catalytic capacity(conversion 72%, selectivity 51.3%) on the Ni-based metasilicate compared with pure one. The obtained heterogeneous Ni-based metasilicate retain durable catalytic activity during five recycling for styrene oxidation and inherit the regulated catalytic performance in the substrate expansion.