Angus Campbell, a crofter at Plocropol, can be found in the 1881 census with his wife Margaret, four years his junior. Their son Alex[ande]r (26) is a general merchant. His other children include Chirsty (24), Murdo (22, fisherman), John (19, fisherman), Angus (17), and two daughters named Cathrine (aged 10 and 7).
Ten years before, the family is picked up in the census of 1871, but their ages appear to be 3 or 4 years younger than you would have anticipated. Angus is at that time a crofter and fisherman, still in the Bays area of Harris. I have not been able to locate Angus Campbell with any certainty in the censuses for 1851 or 1841.
EDIT: Direcleit has kindly added the census entry for 1861 in the comments section.
Going forward, the family is still in Plocropol (no 7) in 1891, although Angus (65) is marked as being born in Lewis, Ross-shire. That is an obvious mistake; he remarked in his evidence that he was a young man around Obbe, South Harris. Of the family, we see Alexander (37) at home, but his brothers Murdo, John and Angus are no longer there. Daughters Christy (33), Catherine (23), Christina (20) and Katie (16) do remain at home. A grandson Angus Campbell (3) has appeared on the scene.
Angus Campbell does not appear to feature in the 1901 census. He passed away on 1 August 1909 at Plocropol at the age of 85, having suffered senile decay. He was the widower of Margaret Mcdonald; she predeceased him in 1901. His parents are named as Alexander Campbell and Chirsty Campbell. The death was reported by Angus's grandson, his namesake Angus Campbell.