Penrhyn, an opponent of trade unions who engaged in frequent disputes with his employees, was called "the best hated employer in Britain".
He was commissioned on 1 March 1860 as captain-commandant of the 1st (Carnarvon) Carnarvonshire Rifle Volunteer Corps, which was largely recruited from his family's Penrhyn Slate Quarry.
A second unit was soon raised from Pennant employees and he was promoted to major in command of the 1st Administrative Battalion of Carnarvonshire Rifle Volunteers.
After that he devoted most of his time and energy to the management of the 26,278 acres (106.34 km2) Penrhyn Estate, which had a rent-roll of £67,000, and the slate quarry at Bethesda which at its peak was estimated to produce £150,000 a year.
An angry debate took place in the House of Commons but Lord Penrhyn would abate none of his conditions, and the men capitulated.
On 9 August 1901, Robert Thomas Jones, raised an urgent discussion on the conduct of the local magistrates in requisitioning cavalry for maintaining peace in the district, but Penrhyn's position was unaffected.
On 13 March 1903, he brought an action for libel against William John Parry, in respect of an article in the Clarion, accusing him of cruelty to his workmen; he received £500 damages and costs.
Penrhyn acted throughout in accordance with what he believed to be stern equity and from a wish to obtain justice for non-union men.
[dubious – discuss] In 1907, he gave his workmen a bonus of 10 per cent, owing to bad weather which had interrupted work at the quarries.