His deputy Thangboi Singto was appointed interim coach.
Under Scottish Bulpin, who took charge in June last year before the start of this I-League season, Lajong could win just three matches out of 17 they have played with six draws and eight losses.
Lajong are not far from the relegation zone, occupying ninth place with 15 points out of 14 teams. They are just one point ahead of Salgaocar, Air India and Sporting Clube de Goa, who are on 10th, 11th and 12th positions respectively.
The Shillong-based side have not won in their last nine matches and had to face the humiliation of 0-6 drubbing at the hands of league leaders Churchill Brothers in a Round 14 match in Goa early this month.
"Shillong Lajong Football Club has relieved Chief Coach Desmond Bulpin of his duties. Assistant coach Thangboi Singto will take charge as interim coach with immediate effect," said club General Secretary Larsing Ming Sawyan in a statement.
Also Read
"The club would like to place on record the valuable contributions of Desmond Bulpin in the youth development system of the club, which we believe will pay dividends in the near future. We thank him for his services and commitment showed to the club. We wish him all the best for the future. Our immediate goal is to concentrate on the next two games and the away game at Salgaocar before the break."
Bulpin was the former coach of English Premier League side Tottenham Hotspur youth team and has been credited for spotting players like former England international Peter Crouch. He was the coach of Philippines senior national team before shifting base to India in 2010 to become coach of AIFF development side (AIFF XI, now Pailan Arrows) on the recommendation of then India coach Bob Houghton.
He was made India Under 23 coach in the later part of 2011 to take charge of the Olympic Games qualifying round campaign.