From the perspective of bond order-length-strength correlation and the local bond averaging approach, we have formulated the number-of-layer resolved Raman shifts of graphene, with quantification of the referential origins from which the Raman shifts proceed and clarification of their origins. It is found that the primary D mode and the secondary 2D mode are dominated by the interaction between a specific atom and its nearest neighbors while the G mode by the dimer interaction, and therefore red shift happens to the D/2D phonons and blue shift to the G mode upon the number-of-layer is reduced.
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