A 26-year-old woman and a 25-year-old man in the same car as the two tots also died in the fatal crash that happened by Hillfarm, Torlundy at about 5.30pm yesterday.
The driver of the second car, a 56-year-old woman was taken to Bedford Hospital, Fort William with what was described as serious but non-life threatening injuries.
Emergency services were made aware of a two car crash involving a Mini Cooper and a Ford Fiesta.
Police Scotland are appealing for information.
Superintendent Simon Bradshaw, said: “Enquiries are continuing into the incident and I would ask anyone with information or dashcam footage who has not yet come forward to please get in touch.”
Anyone with information is asked to contact police on 101 quoting incident 2942 of 20 February.