Born in Papua New Guinea, Segeyaro moved to Cairns, Queensland with his mother at the age of seven. After playing junior football for the Cairns Ivanhoes club, Segeyaro moved to the South Sydney Rabbitohs in 2007. After being cut from the Souths' roster due to disciplinary issues, he returned to North Queensland to play for the Cowboys. Segeyaro was captain of the Cowboys' Toyota Cup team in 2010 and played for the Northern Pride in the Queensland Cup. Segeyaro was selected in the Junior Kangaroos at the end of the 2010 season.
Segeyaro broke into the Cowboys NRL squad in 2011 after undergoing a shoulder reconstruction at the end of the previous season. Segeyaro made his NRL debut in Round 3 against the Melbourne Storm playing off the interchange bench in the Cowboys 34-6 win at 1300SMILES Stadium. In Round 15 against the New Zealand Warriors, Segeyaro scored his first NRL career try in Cowboys 30-10 win at 1300SMILES Stadium. Segeyaro made his first start at hooker in the Cowboys 42-8 Qualifying Finals loss to the Manly-Warringah Sea Eagles at SFS. Segeyaro went on to appear in 19 matches and score 5 tries for the Cowboys the 2012 NRL season. At the end of the season he made his debut for Papua New Guinea in a 36–22 defeat to the Australian Prime Minister's XIII.
On 15 June 2012, Segeyaro announced that he will join the Penrith Panthers on a three-year deal from 2013 to till the end of 2016. In Round 13 against the Gold Coast Titans, Segeyaro suffered an ankle syndesmosis injury in the Cowboys 28-12 loss at Cbus Super Stadium ruling him out until Round 26 in the Cowboys 36-22 win against the Cronulla-Sutherland Sharks at Remondis Stadium. Segayaro played in the Cowboys Week 1 and 2 finals matches. Segeyaro played in 14 matches and scored 3 tries for the Cowboys in the 2012 NRL season.
Segeyaro made his Penrith Panthers club debut in Round 1 against the Canberra Raiders playing off the interchange bench, scoring a try in the Panthers 32-10 win at Penrith Stadium. In Round 24 against the Brisbane Broncos, Segeyaro scored a hatrick in the Panthers 28-12 win at Penrith Stadium. Segeyaro played in all the Panthers 24 matches and scored 10 tries in a stellar debut year for the Panthers in the 2013 NRL season. Injury prevented Segeyaro from representing Papua New Guinea in the 2013 World Cup.
On 22 August 2014, Segeyaro lost his father Iffysoe Segeyaro, who represented the Kumuls, after he died suffering an aneurysm, with Segeyaro missing the Panthers match against the Melbourne Storm at Penrith Stadium and travelling to Papua New Guinea. The Panthers wore black armbands and hold a minute silence in honour of Segeyaro’s father. The Panthers lost the match 24-10. Segeyaro returned for the Panthers in Round 26 against the New Zealand Warriors, scoring a try in the Panthers 22-6 win at Penrith Stadium. Segeyaro finished off the Panthers 2014 NRL season with him playing in 25 matches and scoring 10 tries. On 29 September 2014, at the 2014 Dally M Awards, Segeyaro was named 2014 Dally M Hooker of the Year.
Segeyaro finished off the 2015 season having played in 18 matches and scoring 6 tries for the Panthers. On 26 September, he was called up by club coach and 2015 Prime Minister's XIII coach Ivan Cleary to play against Papua New Guinea. Segeyaro made controversy when he rejected playing for his country of birth and was happy to accept wearing the green and gold jersey in the annual fixture that occurs at the end of the domestic rugby league season. He would go on to receive boos whenever he touched the ball in the match.
On 22 February 2016, Segeyaro was named as the captain of the Panthers 2016 NRL Auckland Nines squad. In Round 1 against the Canberra Raiders, Segeyaro played his 100th NRL career match but unfortunately broken his arm during the Panthers 30-22 loss at Canberra Stadium. After a string of injuries and loss of form, Segeyaro was falling out of favour with Penrith Coach Anthony Griffin and was languishing in the Panthers NSW Cup team. With his future at Penrith fading away, on 23 June 2016, Segeyaro signed an immediate 2-year deal with the Leeds Rhinos, with the Rhinos trading fullback Zak Hardaker to the Panthers. Segeyaro finished the 2016 NRL season with him playing in 4 matches for the Panthers.
Segeyaro made a mid-season move to the Leeds Rhinos in a swap for Zak Hardaker that would see him play for Leeds for the rest of the season. He signed a two-year deal with the Super League club but in December 2016 returned to Australia and announced that due to homesickness he had no intention of returning to the UK. The Leeds Rhinos alleged a breach of contract and were considering legal means.
In March 2017 Leeds agreed a settlement that allowed Segeyaro to join NRL side Cronulla Sharks with immediate effect.