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[Display omitted] • Various Pt shell structures were synthesised on the surface of Pd NCs. • Pt surface facets impact significantly on the mechanism of neutral GOR. • GOR on the stellated Pd@Pt NCs with (2 1 1) facets occurs via a 12-electron patwahy. • Stellated Pd@Pt NCs are the best catalyst for sequential GOR. • Pd NCs with Pt corners having (2 1 0) and (9 5 0) facets enhance transient catalysis. Nanocrystals with high-indexed facets and low-coordinated atoms exhibit promising electrocatalytic activities. Herein, different Pt shell structures on the surface of Pd nanocubes (Pd@Pt NCs) were synthesised by varying the concentration of Pt precursors. The concave Pd@Pt NCs were used as electrocatalysts for neutral glucose oxidation reactions (GORs); the effect of Pt structure on the catalytic performance was studied. In sequential catalysis, stellated Pd@Pt NCs (Pd@Pt SNC) with (2 1 1) facets had an electron transfer number (N e) of 12.69 and a specific activity of 4.69 × 10−9 mol·g·m−2, markedly higher than that of the other concave Pd@Pt NCs. In transient catalysis, Pd NCs with Pt-coated corners (Pd@Pt CNCC) containing (2 1 0) and (9 5 0) facets demonstrated a sensitivity of 11.06 μA·mM−1·cm−2 and a linear analysis range (2.4–10.6 mM). The high recoveries (98.80%–99.85%) and low relative standards (≤1.06%) in the serum sample corroborate the potential of Pd@Pt CNCC as an enzyme-free glucose sensor. [ABSTRACT FROM AUTHOR]