I think you are bypassing a good chunk of off-the-beaten path yet very interesting places between Barcelona and Valencia and further down the Mediterranean coast. Have you considered renting a car as you leave Barcelona to travel south to Valencia and points beyond? I did a road trip in this area over the summer and was pleasantly surprise by the amount of sites and places to see and the the relative lack of tourists, especially foreign ones. This area is known as the Costa Dorada and continues into the Costa del Azahar all the way to Valencia and beyond, it's a land full of ancient olive trees, citrus groves, sandy beaches, lazy beach towns, time-warped castles, and Roman Ruins.
Here are some of my favorite points of interest in the area.
Poblet Royal Monastery - a UNESCO World Heritage Site and still active 12th-century Cistercian monastery. It was a fortified medieval royal residence and contains the unique hanging tombs of the old Kings of Aragon.
Tarragona - ancient seaside town with very good Roman ruins, including an amphitheater, intact aqueduct, and Praetorium Tower, was once the capital of Roman Hispania (modern-day Spain). Tarragona's medieval old town is a delight to explore too.
Les Ferreres Aqueduct - Roman Aqueduct you can walk on top of, a few km from Tarragona.
Sitges - the quintessential posh beach town, 30 min south from Barcelona. Has multiple small sandy beaches. Known for its gay scene, Sitges also has nice historic centre lined with boutique restaurants and shops.
Castillo de Miravet - A large riverside stronghold built by the Knights Templar with commanding views of the countryside. The adjacent medieval village spills down the cliff towards the rivers. A great place to bicycle, kayak, or take a leisurely boat down the Ebro river.
Peñíscola - With its cobbled streets and whitewashed houses, the old town of Peñíscola sits on a big rock that juts out into the sea. The town is dominated by a large Knights Templar castle that looks like something out of the Crusades. Recently, Peñíscola was used as a filming location in the T.V. series Game of Thrones.
Matarraña Region - often referred to as the “Tuscany of Spain”, sprawling vineyards, olive groves, and ancient stone villages. The unspoiled Matarraña region is located in the province of Teruel in southern Aragon, here they speak a dialect of Catalan.
Sagunto Castle (Saguntum) - settlement sacked by Hannibal Barca that led to the Second Punic War. Now an eclectic mix of Roman, Moorish, and Christian fortifications.
Here is my trip report of my road trip to the region - https://community.ricksteves.com/travel-forum/trip-reports/undiscovered-spain-mediterranean-roadtrip-2023
Here are some of my pictures from the road trip - https://photos.app.goo.gl/sMsd6Wz2fydGKYtr5