In 2013, Amala achieved her first commercial success in Telugu cinema. Her first release in 2013, V. V. Vinayak’s directorial Naayak, opposite Ram Charan Teja, went on to be one of the biggest critical as well as commercial successes of the year. Her next film was Puri Jagannadh’s romantic comedy Iddarammayilatho opposite Allu Arjun. Upon release, Amala’s performance was appreciated by the critics. Sangeetha Devi Dundroo of The Hindu commented: “Amala Paul manages to pull off a character that traverses a thin line between being naïve and downright silly. We wish we saw more of her.” Another reviewer, Sasidhar AS from The Times of India commented: “Amala Paul’s characterisation is a delight, and she plays Komali so effectively that you’ll be left wondering who else could have done the role better than her. She was a perfect choice to play a traditional Telugu girl.” She was later seen in A. L. Vijay’s action entertainer Thalaivaa, opposite Vijay, as a police officer. Her last release of the year was the Malayalam film Oru Indian Pranayakatha. The film was a blockbuster at the Kerala box office and she received several awards for her character Irena, including the SIIMA Award for Best Actress – Malayalam consecutively for two years.

In 2014, her first release was Samuthirakani’s Nimirndhu Nil, opposite Jayam Ravi, which was simultaneously shot in Telugu as Janda Pai Kapiraju, in which Nani reprised the role of Jayam Ravi. Her next release Velaiyilla Pattathari, opposite Dhanush was a success in Tamil Nadu and her performance was appreciated.

As early as 2011, when Amala was working on Deiva Thirumagal, she was romantically linked to director A. L. Vijay, but denied that the pair were dating. On 7 June 2014, she got engaged to Vijay at Aluva in Kochi. The couple got married on 12 June 2014 at Mayor Ramanathan Chettiar Hall, Chennai. In 2016, Amala and Vijay filed for a divorce due to disagreement between her and her in-laws on continuing her acting career. They were granted divorce in February 2017. In March 2020, Paul married musician Bhavinder Singh.

In 2015, she appeared in Rajesh Pillai’s Mili, playing the titular role. Her performance in the film was critically acclaimed. She then went on to act with Mohanlal for the second time in Lailaa O Lailaa. Even though it was a big budget film, it didn’t perform well in theatres. In 2016, she signed for four Malayalam films – 2 Penkuttikal, Shajahanum Pareekuttiyum, Ore Mugham and Thoppil Joppan, but left the later two projects due to conflicting schedules. Amala also appeared in a Tamil film Amma Kanakku, playing the mother of a 15-year old. She made her Kannada debut in the film Hebbuli, opposite Sudeep. Hebbuli became a great success in the Karnataka box office. Later, she acted in the Malayalam film Achayans, with Jayaram, which was released in May 2017 and became a commercial success at the box office. In later 2017, she had two releases in Tamil Velaiilla Pattadhari 2 and Thiruttu Payale 2 both did well in the box office. Amala had signed to play lead roles in Malayalam remake of queen and Kayamkulam Kochunni but later opted out of both as she has signed 3 Tamil films for 2018.

In January 2018, Amala was arrested for tax evasion. A crime branch investigation had found that she had registered her luxury car in Puducherry with fake documents. Later, the case was closed citing jurisdictional issues.