From May 2002 to May 2005, Dalić worked as the club's sports director, and during the 2003–04 and 2004–05 seasons he simultaneously acted as assistant coach for Miroslav Blažević.

In the second leg in Varaždin, Dalić nearly created a sensation leading the team to a 5–1 win, but they were one goal short from lifting the silverware.

[7] He resigned in February 2009 after losing two derbies in a row versus fellow capital teams Tirana and Partizani.

At the end of the 2010–11 season under Dalić the club enjoyed the greatest success in its history, qualifying for the King's Cup in the Saudi Professional League.

[11] In the selection, he beat other more famous coaches working in Saudi Arabia at the time, such as Gabriel Calderón, Walter Zenga and Eric Gerets.

[12] On 9 February 2013, he made his managerial debut with Al-Hilal against his old club Al-Faisaly in the semi-final of the 2012–13 Saudi Crown Prince Cup.

[14] On 8 March 2014, Dalić was appointed manager of Al-Ain in the United Arab Emirates after the team had sacked Quique Sánchez Flores.

[19] Dalić won the title of Best Coach of 2014 for his performances; at the end of the first round of the UAE Pro-League, Al–Ain took the first position with one game in hand.

[33] In the return leg, on 12 November, Croatia drew with Greece 0–0, but won 4–1 on aggregate, thus securing a place in the World Cup finals.

[34] Following this, Dalić officially signed a contract with the Croatian Football Federation, running until 30 July 2020, and would reportedly earn around €500,000 per year.

[42] On 21 June, Croatia overwhelmed football heavyweights Argentina, winning by a scoreline of 3–0, with Ante Rebić, Luka Modrić and Ivan Rakitić scoring the goals.

[43][44] The victory led Croatia to a spot in the knockout stage for the first time since the 1998 FIFA World Cup, in which they finished third place.

[45] On 26 June, Croatia topped their group with maximum points following a 2–1 win over Iceland, and drew Denmark in the round of sixteen, advancing after a penalty shootout.

[58] Nevertheless, due to a goalless draw with England in Rijeka on 12 October[59] and a 2–1 defeat in London on 18 November, Croatia were relegated to League B.

[61] Croatia entered their UEFA Euro 2020 qualifying campaign poorly with narrow 2–1 home victories over Azerbaijan and Wales, and an upset 2–1 away defeat to Hungary.

On 16 November 2019, in their last qualifying match, Croatia beat Slovakia 3–1 in Rijeka, topping the group and securing their place at the finals.

[67][68] Croatia entered their 2020–21 UEFA Nations League campaign poorly, losing heavily to Portugal and France away, 4–1 and 4–2 respectively.

[76][77][78] In the 2022 World Cup, Dalić led Croatia to their second consecutive semi-final and third in total, after beating Brazil on penalties in the quarter-finals.

They defeated the host Netherlands 4–2 and won a silver medal, losing the final to Spain in a penalty shootout after the score was 0–0.

Dalić is widely regarded as the greatest coach in the history of the Croatian national team due to his success achieved at multiple World Cups, consisting of a runner-up and a third place finish.