Kaifi wrote the songs for Chetan Anand's war film Haqeeqat (1964), which featured iconic songs like Kar Chale Hum Fida. His column Chunav Charcha, which appeared in the Urdu edition of Blitz, was a striking example of how he blended political analysis with literary flair. Usually appearing in a run-up to the elections, these articles explored the promises, propaganda and posturing of the candidates with a fine-tooth comb. As opposed to dry political commentary, Chunav Charcha carried the cadence and razor-sharpness of Kaifi Azmi's verse. Alongside this, Nayi Gulistan was Kaifi Azmi's literary column published in the Urdu journal Blitz during the 1960s and 70s. As a prominent figure of the Progressive Writers' Association, Kaifi utilised the platform to challenge feudalism, communalism and the hypocrisies of the growing Indian middle-class, the burgeoisie. In a series of polemical essays and articles, he addressed worker's rights, the exploitation of peasants and labourers, communal polarisation and the pressing need for a modern, socialist vision for India.

He wrote the song lyrics for the soundtrack of the Khwaja Ahmad Abbas' Saat Hindustani (1969), which won him the National Film Award for Best Lyrics.

He penned the entire script in verse for Chetan Anand's Heer Raanjha (1970), a unique achievement in Hindi cinema. The dialogues rhymed with each other, and were formatted like poetry. In a sense, the script was one big poem, composed largely by Kaifi Azmi. His next significant song was in Pakeezah (1972), Kamal Amrohi's magnum opus, where he wrote the sensational Chalte chalte yun hi koi mil gaya tha..

M.S. Sathyu's Garm Hava (1973) was named after Kaifi's poem 'Makan' which had appeared in the film Sone ki Chidiya.. Shama Zaidi and Kaifi cowrote the screenplay of Garm Hava, basing it on Ismat Chugtai's short story about the patriarch of a Muslim family grappling with the question of whether to migrate to Pakistan as the Partition unfolded. All three — Kaifi, Shama, and Sathyu — were associated with the Indian People's Theatre Association (IPTA), and the film reflects the wordview and concerns of that generation, conveyed through Kaifi's lines. A brain haemorrhage on 8 February, 1973 left him partially paralysed, with his left hand and leg permanently impaired. Yet, rather than retreat into hopelessness, he chose to leave behind the comforts of Bombay and return to Mijwan, his birthplace.

In 1974, Kaifi Azmi was conferred the Padma Shri for his contribution. Awara Sajde, his third poetry collection, came out the same year. The book won him a Sahitya Akademi Award in 1975. Shyam Benegal's seminal film Manthan (1976) had dialogues written by him, on a screenplay by Vijay Tendulkar. Kaifi wrote three iconic songs for Mahesh Bhatt's Arth (1982): Jhuki jhuki si nazar, Tum itna jo muskura rahe ho, and Koi yeh kaise bataye.

Kamal Amrohi's Razia Sultan (1983) featured a song written by him alongside several by Jan Nisar Akhtar, Javed Akhtar's father. In this phase, he collaborated often with Bappi Lahiri on films like Bhavna (1984), Hum Rahe na Hum (1984) and Shart (1986), most of which featured Ghazals, a deviation from Lahiri's usual expertise. Kaifi wrote the only song Itne baazu itne sar in the Amitabh Bachchan-strarrer Main Azaad Hoon (1989). Written as a protest song, the number harks back to his IPTA days. He returned his Padma Shri in 1986, objecting to a politican making derogatory remarks against Urdu. The Babri masjid incident made him write the poem Doosra Banwas, implying that the tragedy was tantamount to a second exile that Lord Ram had to endure. Kaifi's collaborations with Mahesh Bhatt continued through the 90s: Phir Teri Kahani Yaad Ayee (1993) and Tamanna (1996). The latter includes Kaifi's iconic poem "Aurat". In 1993, he featured in his only major acting role in Saeed Mirza's Naseem (1995).

Kaifi Azmi passed away on May 10 2002 in Mumbai due to cardiac and respiratory complications, aged 83. His Communist Party membership card was buried with him as per his wishes.