Atomic-level　manufacturing　is　fundamentally　concerned　with　the　precise　removal,　addition,　and　migration　of　material　at　the　atomic　and　close-to-atomic　scale　(ACS).　Tip-based　electrochemical　deposition,　a　quintessential　ACS　electrochemical　additive　manufacturing　technique,　offers　promising　prospects　for　achieving　bottom-up　fabrication　of　metallic　micro/nano　structures.　However,　the　complex　physicochemical　reactions　involved　in　electrodes　lead　to　a　limited　understanding　of　the　mechanisms　underlying　atomic　electrodeposition　and　structural　evolution.　For　the　first　time,　this　study　proposes　electric　double-layer　controlled　electrochemical　kinetics　and　investigates　the　effect　of　direct　current　(DC)　and　pulse　current　(PC)　on　nickel　atomic　electrodeposition　using　molecular　dynamics　(MD)　simulations.　The　findings　reveal　that　compared　to　DC　electrodeposition,　PC　electrodeposition　results　in　more　orderly　deposition　morphology,　improved　surface　smoothness,　reduced　dislocation　density,　and　lower　crystal　distortion,　with　these　effects　being　particularly　pronounced　under　low　pulse　duty　ratio　conditions.　In　addition,　the　pulse　frequency　significantly　influences　the　morphology　and　structure　of　the　deposit.　The　high　pulse　frequency　yields　smoother　surfaces　with　local　protrusions,　while　the　low　frequency　favors　the　formation　of　orderly　and　dense　structures　excepting　slightly　increased　roughness.　This　study　provides　critical　insights　into　understanding　the　microscopic　mechanisms　of　atomic-scale　electrodeposition　processes　and　achieving　atomically　controlled　tip-based　electrochemical　additive　manufacturing　of　micro/nanodevices.