Hui decided to pursue dentistry after job shadowing at his uncle's dental clinic for two weeks.

On 4 March 2011, Alfred Hui signed a contract with Stars Shine International (星煥國際) as a singer.

Hui represented Hong Kong to participate in the ABU TV Song Festival 2012, which was scheduled to take place at the KBS Concert Hall, in Seoul, South Korea, on 14 October 2012.

[6][better source needed][7] His third studio album Grandit (長大), meaning "growing up" in French, was released in December 2012.

The single "The Ode of Youth" (青春頌), which echoes the theme of the song "Grandit" and serves as the conclusion of the album, received critical acclaim.

[8] On 31 October 2013, Alfred Hui followed Herman Ho Chit-to (何哲圖), Chief Executive Officer of Stars Shine (星煥國際), to join the Voice Entertainment Group Limited (星夢娛樂).

On 28 and 29 December 2013, The Times – Alfred Hui Solo Concert 2013 (許廷鏗時光演唱會2013) was organized at the Star Hall (匯星) of Kowloonbay International Trade & Exhibition Centre (九龍灣國際展貿中心).

On December 7, 2014, Alfred Hui's two singles "Chain" and "Blessing" ranked second and tenth respectively on the Jade Solid Gold music chart.

In 2015, Alfred Hui released Colour By Numbers and Watermark albums in January and December respectively, each with 11 songs.

This was his first time directing his own music video, starring former ATV veteran actor Nina Paw.

Since September 1, he has briefly participated in the cartoons drawn by cartoonist YY in Headline Daily every Thursday.

Songs included "Blue" (藍血人), "Miraculous Journey", "OCD" (強迫症進行曲) and "ADD" (大雄胖虎綜合症).

[12] In August 2018, Hui collaborated with RubberBand's Mau Hou Cheong and released a new single "Spare A Listen" (停半分鐘聽一闋歌) as a tribute to Cantopop.

In November, he released a new song "Innocence" (白紙), which was composed and produced by his friend Yu Yat Yiu.

[13] In the same year, Hui served as one of the judges in the fourth round of ViuTV's King Maker III.

In January 2022, local media reported that ten Canto-pop singers and groups had been put on a blacklist of government-funded broadcaster RTHK, with radio DJs having been ordered not to play their songs.