According to the United States Census Bureau, the township has a total area of 41.7 square miles (108.0 km²), of which, 41.6 square miles (107.8 km²) of it is land and 0.1 square miles (0.2 km²) of it (0.19%) is water.
Smithfield Township is bordered by Ridgebury and Athens Townships to the north, Ulster Township to the east, Burlington and West Burlington Townships to the south and Springfield Township to the west.
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