Paylan was among the few Armenians elected to the Grand National Assembly of Turkey and served for two consecutive terms in 2015–2018 and 2018–2023, representing Istanbul and Diyarbakir.

His grandparents on both sides were survivors of the 1915 Armenian deportation and Paylan said “I grew up in a household with my grandmother, who an orphan who had lost her entire family.

The only place that would heal the wound of Armenian nation is this parliament.” Paylan submitted a similar proposal in 2022 but was harshly criticized by the Turkish President, Recep Tayyip Erdogan, and the leader of the nationalist MHP, Devlet Bahceli.

In 2022, Paylan went on a tour of eastern Turkey to identify and document churches and synagogues in the countryside facing destruction and ruin, including the Surp Bartholomes in Baskale, Van, dating back 1600 years.

Paylan made videos of these historic monuments to raise awareness and called on Ministry of Culture and Tourism to preserve the buildings.

Paylan called for a government investigation into reports in 2019 that at a Turkish summer camp for girls, kids were encouraged to shout “death to Jews”.

Paylan highlighted discrimination against non-Muslim minority communities during his time in the parliament, including the 6–7 September 1955 pogroms against Jewish, Greek, and Armenian communities in Istanbul and sought to submit a bill to the parliament to declare that date “Memory Day.” He also called for the removal of street names that honored the perpetrators of the Armenian deportations, most significantly Talat Pasha, equating it to calling streets in Germany in memory of Adolf Hitler.

Paylan was physically attacked on 2 May 2016 inside the Turkish parliament during a subcommittee meeting on constitutional reform and suffered minor injuries.

Paylan filed legal complaint about the advertisement and wrote in an op-ed in the New York Times, “As an Armenian from Turkey and a descendant of deportation survivors, I know very well the meaning of this message.” On 17 March 2021, the State Prosecutor for the Court of Cassation, Bekir Şahin, filed a lawsuit[13] before the Constitutional Court demanding in an indictment that the pro-Kurdish HDP to be shut down due to the party's alleged organizational links with the Kurdistan Workers' Party (PKK).

[16][17] At the 700th meeting of Saturday Mothers, Paylan fought off a police effort to detain the demonstrators, including journalist Ahmet Şık and the son of Hrant Dink.

"[18] On 1 November 2022, in Yerevan, Paylan made an impromptu visit after meeting Armenia's prime minister Nikol Pashinyan earlier that day.