After leaving NUS Wales, Smith worked for ten months as an assistant at the international development organisation United Purpose.

She later worked as an eight-month temporary political researcher to Jill Evans at the European Parliament, before returning to a role at United Purpose apparently based in New York City for eight months.

[4] Following her nomination, Smith said that she would "[fight] for a fair deal for Wales" and "work to inspire the next generation of women to take an active role in our communities and our nation".

This was a result of a Plaid Cymru National Executive Committee decision, announced in advance of the vote, that nominees for peerages would alternate between women and men.

[4] Some Plaid Cymru members criticised her appointment as undemocratic and unfair, and took issue with her lack of experience compared to her rival candidates.

[12] Speaking on a BBC Newscast podcast with Laura Kuenssberg and Paddy O'Connell, Smith revealed that she would take "of Llanfaes" as her territorial designation.