Through his influence, Sir Edward gained various positions, including Master of the Mint, Member of Parliament for Westminster and Lord President of Munster.

In October 1617, he succeeded Sir Richard Martin as Master of the Mint (until 1623), and in November 1618 he became comptroller of the Court of Wards.

In the same month he was sent to Frederick V, Elector Palatine, to say that assistance would be given to him, but only on condition that he entered into an agreement to relinquish the crown of Bohemia.

His conduct was vindicated in the inquiry by the House of Lords in June, and Villiers was allowed to resume his seat in the Commons.

In September he was again sent to the Elector Frederick, then serving with the Dutch army, to persuade him to withdraw from it and submit to the Holy Roman Emperor.

On 23 September 1622, he was granted a lease of the customs and subsidies on gold and silver thread on condition of surrendering the mastership of the mint, but the latter office was restored to him in July 1624.

Eleanor Villiers was a maid of honour in the household of Henrietta Maria, and performed in the masque The Shepherd's Paradise.