The products are the result of a two-year global collaboration on a range of items, from jeans to shirts. Nine one-off hand-painted bikes have also been styled by the British designer.
The bikes will be exhibited around the country at trade shows and design exhibitions and will feature in a window display as part of Harrods' "Truly British" initiative.
Triumph has launched a website, created by Bristol-based digital agency E3, to promote the collaboration.
Paul Smith has also teamed up with HP Sauce to update the brand's image. It will launch limited-edition redesigned bottles with trademark Paul Smith stripes, which will go on sale exclusively in Harrods.
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